We systematically explored PEG alternatives by synthesizing a combinatorial library of nine copolymers composed of three hydrophilic monomers including oligo(ethylene glycol) methyl ether methacrylate and 2-(methylsulfin...We systematically explored PEG alternatives by synthesizing a combinatorial library of nine copolymers composed of three hydrophilic monomers including oligo(ethylene glycol) methyl ether methacrylate and 2-(methylsulfinyl)ethyl methacrylate and three hydrophobic monomers. These copolymers were evaluated for their hydrophobicity by reversed-phase chromatography and LCST behavior, and for their biodistribution. Extended hydrophilic brushes enhanced blood retention and tumor accumulation. For copolymers with the longest brushes, hydrophobic side chains minimally influenced kidney accumulation, whereas kidney accumulation of copolymers with medium-length brushes was strongly influenced. Liver accumulation of the copolymers was hardly affected by the hydrophobic side chain, except for the copolymer with the longest brushes and the most hydrophobic side chains, which showed increased liver accumulation. This study highlights the critical role of hydrophilic brushes and hydrophobic side chains in modulating biodistribution of polymeric carriers and provides a foundation for rational design of drug delivery systems.
Multicomponent reactions (MCRs) enable efficient construction of multifunctional materials, with iminoboronate chemistry offering attractive pH and redox responsiveness for smart biomaterials. However, their poor kinetic...Multicomponent reactions (MCRs) enable efficient construction of multifunctional materials, with iminoboronate chemistry offering attractive pH and redox responsiveness for smart biomaterials. However, their poor kinetic stability under aqueous dilution and elevated CO levels limit biomedical applications. Herein, we address this challenge by embedding iminoboronate linkages within supramolecular assemblies, where nanoconfinement modulates their kinetic behaviors. The hydrophobic microenvironment of the supramolecular micellar core effectively restricts water accessibility to the iminoboronate moieties, converting the inherent kinetic instability into assembly-dependent and environment-regulated stability. By varying amine derivatives and natural polyphenols, a series of multicomponent supramolecular micelles were constructed. In cellular studies and postoperative skin cancer models, multifunctional micelles coloaded with doxorubicin and epigallocatechin gallate exhibited a synergistic therapeutic profile, effectively suppressing tumor recurrence while simultaneously promoting wound healing. This work establishes supramolecular confinement as a general strategy to stabilize kinetically labile MCR-derived linkages, expanding the biomedical potential of iminoboronate chemistry.
Electrostatic interactions play a central role in governing the swelling and mechanical properties of protein-based hydrogels, yet their influence near the isoelectric point (pI) remains poorly understood in chemically c...Electrostatic interactions play a central role in governing the swelling and mechanical properties of protein-based hydrogels, yet their influence near the isoelectric point (pI) remains poorly understood in chemically cross-linked protein hydrogels. Herein, we investigated the pH-dependent swelling and mechanics of a chemically cross-linked recombinant protein hydrogel constructed from GRG5RG4R (pI ≈ 4.6), an engineered elastomeric protein consisting of folded globular domains GB1 interspersed with unstructured resilin sequences. We found that at pI, the hydrogel equilibrated in NaCl solution not only showed the smallest swelling ratio due to minimized electrostatic repulsion and Donnan osmotic pressure at charge neutrality but also exhibited the highest Young's modulus and toughness. These results demonstrated the feasibility of tuning the electrostatic interactions to engineer stiff and tough protein hydrogels, a long-standing challenge in material engineering. Moreover, in citrate and sulfate buffers, while the hydrogel displayed the smallest swelling ratio at the pI, the maximum Young's modulus was observed at pH 3, which is below pI, despite increased swelling. This result demonstrated the decoupling of hydrogel's swelling and stiffness. We propose that bivalent anions interact with clustered cationic surface patches of GB1 domains, acting as a secondary ionic cross-linking to enhance the network stiffness. These findings highlight the feasibility of using pH and citrate as mechanisms to tune hydrogel mechanics without altering network chemistry.
Myocardial infarction (MI)-induced heart failure is challenging because of poor cardiac self-repair and adverse remodeling. Hydrogel-based cardiac patches require integrated mechanical, electrical, adhesive, biocompatibl...Myocardial infarction (MI)-induced heart failure is challenging because of poor cardiac self-repair and adverse remodeling. Hydrogel-based cardiac patches require integrated mechanical, electrical, adhesive, biocompatible, and biodegradable properties that remain difficult to achieve. Here, we report that a polysaccharide-based hydrogel patch, i-HEBioPEC, is realized by deliberately further dynamically interlocking an already highly entangled biopolyelectrolyte complex (HE-BioPEC) hydrogel network in situ via a chitosan and EDC/NHS coupling, respectively, inducing a physical bridging and chemical cross-linking synergistic interlocking mechanism. The patch enables on-demand cardiac repair through in situ tissue interlocking, exhibiting myocardium-like strain-stiffening, high toughness, fatigue resistance, tunable strength, and excellent biocompatibility, antimicrobial, and hemostatic performance. In MI rats, i-HEBioPEC effectively suppressed left ventricular dilation and adverse remodeling, improving the cardiac function. Notably, treated rats developed thinner, more mature scars with better functional recovery, indicating the active guidance of favorable repair. This work provides a new design strategy for multifunctional cardiac patches.
Conductive hydrogels possess remarkable advantages when employed as electrode materials for triboelectric nanogenerator (TENG)-based sensing applications. Nevertheless, hydrogel electrodes suffer from critical limitation...Conductive hydrogels possess remarkable advantages when employed as electrode materials for triboelectric nanogenerator (TENG)-based sensing applications. Nevertheless, hydrogel electrodes suffer from critical limitations under low-temperature environments, including increased brittleness and inferior self-healing capability, as well as conductivity degradation caused by the crystallization of free water within the gel matrix. To address these challenges, we developed a eutectogel electrode via rational design of a ternary polymerizable deep eutectic solvent, incorporating chitosan as a reinforcing and conductive secondary network, and integrating extensive hydrogen bonding interactions. The optimized eutectogel (CPD) exhibited a toughness of 0.25 MJ m, a conductivity of 0.25 mS cm, and rapid self-healing ability. Notably, it retained 92% of its room-temperature conductivity, and its mechanical properties remained nearly unchanged at -80 °C. The assembled CPD-TENG generated an open-circuit voltage of 1.3 V in a single electrode mode at room temperature and maintained 1.2 V at -80 °C, which significantly surpassed the low-temperature stability of conventional hydrogel-based TENGs. Moreover, the CPD-TENG-based sensor with self-powered capacity could precisely monitor joint movements, facial expressions, and human locomotion at both room temperature and -20 °C. Overall, this work provides a feasible strategy for developing reliable self-powered sensors for extreme low-temperature applications.
Effective delivery of hydrophobic photosensitizers across complex biological barriers (e.g., superhydrophobic surfaces) for systemic therapeutic action remains a formidable challenge in supramolecular chemistry and mater...Effective delivery of hydrophobic photosensitizers across complex biological barriers (e.g., superhydrophobic surfaces) for systemic therapeutic action remains a formidable challenge in supramolecular chemistry and materials science. Herein, we developed a fluidic supramolecular coacervate platform assembled by liquid-liquid phase separation (LLPS) that spontaneously assembles cationic conjugated polymer photosensitizers with biobased poly(thioctic acid) derivatives into dynamic coacervates (). The fluidic exhibits strong adhesion and deposition on hydrophobic plant surfaces, ensuring excellent retention and efficacy under agricultural conditions. demonstrates remarkable photodynamic antibacterial activity, completely eradicating pv. under white light irradiation. Under natural light, effectively treats rice bacterial blight in vivo and can enhance rice defense by modulating antioxidant enzyme systems. Additionally, leveraging the intrinsic fluorescence of the conjugated backbone, we demonstrate the self-reporting capability of the system, visualizing its uptake by roots and subsequent systemic translocation via vascular bundles to leaves─a feat rarely achieved by hydrophobic photosensitizers. This work presents a paradigm for designing fluidic supramolecular materials to overcome biological barriers, offering a potent strategy for sustainable, pesticide-free bioprotection.
G-quadruplex-based nanowires (G-wires) are promising candidates for high-performance photonic and electronic nanomaterials, yet their utility is restricted by the discontinuous phosphodiester linkages inherent in the cur...G-quadruplex-based nanowires (G-wires) are promising candidates for high-performance photonic and electronic nanomaterials, yet their utility is restricted by the discontinuous phosphodiester linkages inherent in the current assembly methods. These discontinuities impair structural stability, limit axial growth, and compromise the long-range energy transfer efficiency. Herein, by employing hairpin-structured splint strands to template the high-yield cyclization of poly(dC) DNA, we enable rolling circle amplification to produce ultralong poly(dG) DNA that spontaneously self-assembles into micrometer-scale G-wires with a continuous phosphate backbone. Furthermore, a nucleic acid-specific fluorescent probe, thiazole orange (TO), showed a highly efficient long-range energy transfer through G-wires, compared with double-stranded DNA (dsDNA) and G-quadruplex monomers.
Periodontitis requires both inflammation suppression and bone regeneration, yet temporal coordination remains challenging. A core-shell nanofibrous membrane (ICA-PCL@ASTA-PLGA) was fabricated by coaxial electrospinning,...Periodontitis requires both inflammation suppression and bone regeneration, yet temporal coordination remains challenging. A core-shell nanofibrous membrane (ICA-PCL@ASTA-PLGA) was fabricated by coaxial electrospinning, with an astaxanthin (ASTA)-loaded poly(lactic--glycolic acid) (PLGA) shell and an icariin (ICA)-loaded polycaprolactone (PCL) core for sequential drug delivery. Differential degradation enabled rapid initial ASTA release and sustained ICA release over 8 weeks, providing early anti-inflammation followed by osteogenesis. This sequential release drove macrophage polarization from M1 to M2, downregulating proinflammatory and upregulating reparative factors. ASTA inhibited inflammation, while ICA promoted osteogenic gene expression and matrix mineralization, with temporally controlled synergy. These outcomes align with ASTA modulating NF-κB and ICA activating MAPK pathways, as previously reported. In a rabbit periodontitis model, the membrane significantly improved the immune microenvironment and alveolar bone regeneration, outperforming single-drug-loaded scaffolds. This material-guided sequential delivery strategy integrates immunomodulation and osteogenesis, highlighting "material-guided temporal pharmacology" as a paradigm for treating inflammatory tissue defects.
Melanoma is one of the most lethal cancers in the clinic; cationic peptides have shown great potential in the treatment of melanoma. The large pore volume and high specific surface area of mesoporous silica nanoparticles...Melanoma is one of the most lethal cancers in the clinic; cationic peptides have shown great potential in the treatment of melanoma. The large pore volume and high specific surface area of mesoporous silica nanoparticles (MSNs) allow for efficient loading of drugs, while surface-functionalized MSNs can further improve drug stability and carrier targeting. Polydopamine (PDA) coating is an effective surface modification method that provides an additional protective layer to prevent premature drug release during delivery and can prolong the treatment time. Hyaluronic acid (HA) is a commonly used tumor-targeting molecule that binds to HA receptors on the surface of tumor cells, thereby facilitating drug internalization and enhancing the therapeutic effect of the drug. In this paper, the cationic short peptide RKIIIRW, which can effectively inhibit B16F10 cells, was successfully screened by solid-phase synthesis combined with MTT assay and cell membrane chromatography. By combining the cationic short peptide RKIIIRW with MSNs and further surface modification with PDA coating and HA targeting molecules, a nanodrug delivery system with targeted and controllable release characteristics was prepared. This drug-delivery system enhances the efficacy of cationic short peptides while minimizing side effects, offering a more effective therapeutic strategy for melanoma.
Water is indispensable to life and plays a central role in biological functions. In this study, glycopolymers with distinct backbones (acrylamide or acrylate) and linker lengths (methylene or ethylene) were synthesized v...Water is indispensable to life and plays a central role in biological functions. In this study, glycopolymers with distinct backbones (acrylamide or acrylate) and linker lengths (methylene or ethylene) were synthesized via RAFT polymerization to investigate their hydration states. Thermal analysis revealed that glycopolymers with an acrylamide backbone retained more hydration water than those with acrylate backbones. This trend was consistently supported by terahertz spectroscopy and molecular dynamics simulations. In addition, the amount of hydration water increased with increasing linker length. Hemagglutination inhibition assays showed that acrylate-type glycopolymers exhibited markedly higher binding affinity for concanavalin A than their acrylamide-type counterparts across all degrees of polymerization. Importantly, these results reveal a clear inverse correlation between the amount of hydration water and binding affinity, indicating that excessive hydration hinders lectin recognition.
Feng C, Jiang X, Shao Q
… +3 more, Pang Q, Jing X, Yan L
Biomacromolecules
· 2026 Jun · PMID 42381256
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In recent years, with the rapid progress in bioinspired and self-assembly technologies, vesicles that mimic cell membranes have attracted growing research interest. Among them, polymersomes prepared from natural or biode...In recent years, with the rapid progress in bioinspired and self-assembly technologies, vesicles that mimic cell membranes have attracted growing research interest. Among them, polymersomes prepared from natural or biodegradable polymers have emerged as a key focus in biomedicine due to their excellent stability, superior biocompatibility, and low immunogenicity. In particular, permeable polymersomes, as highly biomimetic systems, possess a double-layered membrane structure that enables efficient substance and energy exchange with the external environment, closely resembling natural cell membranes. The entanglement of polymer chains combined with the permeable membrane structure confers outstanding mechanical stability and enhanced permeability, allowing small molecules to pass through while retaining macromolecules inside the vesicle cavity. These unique properties endow permeable polymersomes with broad application potential in drug delivery, diagnostic imaging, and nanoreactors. Given this background, this review summarizes the preparation methods of permeable polymersomes and their recent advances in biomedical applications.
Biomacromolecules
· 2026 Jun · PMID 42377109
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The field of lignin-based polymeric materials is undergoing rapid development, driven by increasing sustainability demands. However, progress in lignin-derived materials is often pursued from different disciplinary persp...The field of lignin-based polymeric materials is undergoing rapid development, driven by increasing sustainability demands. However, progress in lignin-derived materials is often pursued from different disciplinary perspectives─biomass chemistry, organic synthesis, and polymer materials science─using field-specific metrics, resulting in fragmented knowledge. This Perspective examines the lignin-to-materials pathway by connecting advances in the conversion of lignin into platform molecules, their transformation into monomers, and the synthesis of polymeric materials through representative examples. We perform rough estimates of sustainably available lignin streams and compare them with current polymer production, indicating that lignin could potentially supply aromatic monomers at scales comparable to existing markets. Through analysis of key literature on lignin-to-monomers and monomers-to-polymer strategies, we identify critical directions for lignin-to-materials development. These include refinery concepts that utilize complex lignin-derived substrates as primary building blocks, prioritizing the use of their inherent functionality before stepwise defunctionalization, and adopting application-driven materials design, in which the requirements of a target application guide monomer and polymer selection rather than attempting to reproduce the molecular structures of the petroleum-derived polymers currently used for those applications.
Biomacromolecules
· 2026 Jun · PMID 42376978
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Herein, we report degradable cationic polyesters combining pH responsiveness with tunable, anion-induced UCST phase behavior in aqueous media under mildly acidic and physiologically relevant pH conditions, accompanied by...Herein, we report degradable cationic polyesters combining pH responsiveness with tunable, anion-induced UCST phase behavior in aqueous media under mildly acidic and physiologically relevant pH conditions, accompanied by reversible self-coacervation. These main-chain polyesters feature ionizable amine side groups paired with Cl (PE-Cys-Cl) or BF (PE-Cys-BF) counterions, enabling UCST transitions triggered by NaCl, NaBF, and notably by the pharmaceutically relevant anion salicylate (SAL). Cloud point temperature was tuned over a broad range of 8-91 °C by controlling anion type, pH, polymer concentration, and the anion-to-cation repeat unit ratio (A/CRU). Mechanistic studies revealed liquid-liquid phase separation into dynamic, water-rich coacervate droplets. Importantly, the hydrolytic degradation was strongly counterion-dependent, with PE-Cys-Cl exhibiting substantial degradation under physiological conditions compared to low-molecular-weight PLLA, whereas the more hydrophobic PE-Cys-BF polymer remained largely unchanged. These materials provide a versatile proof-of-concept platform for anion-triggered UCST phase separation, opening opportunities in responsive coacervation, anion sensing, and drug delivery related applications.
Biomacromolecules
· 2026 Jun · PMID 42372109
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Lignin contains persistent free radicals (PFRs) stabilized by restricted molecular mobility in a glassy state. Herein, we investigate quenching effects in softwood kraft lignin PFRs by solvation and thermal treatment. El...Lignin contains persistent free radicals (PFRs) stabilized by restricted molecular mobility in a glassy state. Herein, we investigate quenching effects in softwood kraft lignin PFRs by solvation and thermal treatment. Electron paramagnetic resonance (EPR) spectroscopy and temperature-modulated differential scanning calorimetry (TM-DSC) were used to characterize changes. Room-temperature methanol or acetone swelling reduced the paramagnetic signal to 48% and 71% of the original intensity. Similarly, heating lignin above its glass transition temperature () mobilized trapped radicals, leading to their recombination and the depletion of the EPR signal. Both heating and solvent swelling induced a transition from carbon- to oxygen-centered radicals (-value 2.0016 → 2.0033), but only heating caused cross-linking that increased the by approximately 15 °C. Ultimately, overcoming the restricted mobility of the glassy state, whether chemically or thermally, is the primary driver for quenching persistent radicals in kraft lignin.
Mitra H, Nakate P, Stevenson M
… +1 more, Ardekani AM
Biomacromolecules
· 2026 Jun · PMID 42371946
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Efficient drug delivery using nanoparticles (NPs) depends on their ability to diffuse through biological tissues. The extracellular matrix (ECM) poses a key transport barrier, directly influencing biodistribution, cellul...Efficient drug delivery using nanoparticles (NPs) depends on their ability to diffuse through biological tissues. The extracellular matrix (ECM) poses a key transport barrier, directly influencing biodistribution, cellular uptake, and therapeutic efficacy. A primary transport regulator is hyaluronic acid (HA), a major ECM polysaccharide forming a viscoelastic network. Changes in HA concentration alter ECM effective viscosity, while steric obstruction and hydrodynamic drag hinder nanoscale NP mobility. Because HA molecular weights and concentrations vary widely across ages, tissues, and pathologies, we investigated NP diffusion in diverse HA polymer mixtures using dynamic light scattering (DLS). These experiments were complemented by coarse-grained molecular dynamics (CG-MD) simulations. We observed anomalous NP diffusion strongly dictated by the particle-to-network size ratio, particularly in high-molecular-weight mixtures. This transport is governed by the local effective viscosity. Our work establishes a simulation-coupled predictive framework of NP diffusion within specific ECM environments.
Biomacromolecules
· 2026 Jun · PMID 42370992
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Bacterial cellulose (BC) hydrogels produced by species hold considerable promise for a wide range of applications owing to their exceptional mechanical properties, biocompatibility, and biodegradability. Achieving preci...Bacterial cellulose (BC) hydrogels produced by species hold considerable promise for a wide range of applications owing to their exceptional mechanical properties, biocompatibility, and biodegradability. Achieving precise control over their structural and mechanical characteristics is crucial for the engineering of BC-based materials. In this study, we investigated the formation dynamics and structural features of BC hydrogels, emphasizing the complex interplay between cellulose nanofibril secretion and bacterial motility. Comprehensive tracking of bacterial movement during hydrogel formation has validated mechanisms underlying the development of branching and merging junctions, which are key elements that define the network's physical properties. Additionally, we observed the emergence of vortex-lattice and chiral-nematic structures during hydrogel development, depending on bacterial and cellulose densities. These insights contribute to a fundamental understanding of bottom-up 3D fabrication of BC hydrogels that harness the collective behavior of cellulose-producing bacteria.
Burgio C, Giron MD, Ortega-Muñoz M
… +2 more, Lucena D, Salto R
Biomacromolecules
· 2026 Jun · PMID 42363882
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To generate drug-targeting agents with a modular and efficient design for disease treatments, including cancer, we used protein coil-coiled dimerization motifs to eliminate the need for chemical conjugation techniques, g...To generate drug-targeting agents with a modular and efficient design for disease treatments, including cancer, we used protein coil-coiled dimerization motifs to eliminate the need for chemical conjugation techniques, generating a versatile theranostic system: a targeting moiety genetically fused to an E coil and a fusion protein of maltose-binding protein and a monomeric streptavidin that includes a K coil. The system can be directed to other targets by changing the targeting moiety. The second component enables simultaneous binding to two different ligands (maltosylated or biotinylated). We tested the system using a truncated human Galectin-3 as the targeting moiety, which binds to β-galactoside-containing oligosaccharides overexpressed on the plasma membranes of tumor cells, and biotinylated doxorubicin as the cargo molecule. experiments using cell lines that express or do not express Galectin-3 ligands and mouse xenografts demonstrated the system's capability, specificity, and flexibility.
Wang C, Wang J, Huang Y
… +11 more, Lu C, Wang H, Shi G, Zhang Q, Guo C, Zeng L, Song C, Li J, Duan B, Li J, Chang C
Biomacromolecules
· 2026 Jun · PMID 42363874
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Resorbable fracture fixation materials are currently gaining widespread attention due to their ability to avoid the second surgery and stress shielding. Inspired by the structure of the crab shell, herein, we propose hig...Resorbable fracture fixation materials are currently gaining widespread attention due to their ability to avoid the second surgery and stress shielding. Inspired by the structure of the crab shell, herein, we propose high-strength resorbable screws composed of β-tricalcium phosphate (β-TCP) and chitin as orthopedic implants. The incorporation of β-TCP into the chitin matrix not only improved the mechanical performance of the screws but also endowed them with osteogenic activity. The resulting chitin/β-TCP screws exhibited high flexural strength (up to 297 MPa) and tensile strength (up to 257 MPa), comparable to cortical bone. The chitin/β-TCP screws had favorable biocompatibility , which effectively promoted the adhesion of BMSCs and the expression of osteogenesis-related genes (RUNX2 and OCN), thereby facilitating bone healing. Importantly, the assessment of the rat femoral condyle indicated that the chitin/β-TCP screws were firmly fixed within the bone tunnel without inflammatory response and promoted the formation of new bone tissue during degradation. This work provides a biomimetic strategy for designing polysaccharide-based screws with significant potential applications in fracture internal fixation and anterior cruciate ligament reconstruction.
Scarpelli F, Tatli B, Koptelova A
… +5 more, Hirsch M, De Rose R, Brück WM, Crispini A, Abitbol T
Biomacromolecules
· 2026 Jun · PMID 42361203
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Cellulose nanocrystal (CNC)-based materials are promising sustainable alternatives for numerous applications, and enhancing their mechanical robustness while imparting antimicrobial activity could further broaden their u...Cellulose nanocrystal (CNC)-based materials are promising sustainable alternatives for numerous applications, and enhancing their mechanical robustness while imparting antimicrobial activity could further broaden their utility. Here, the Ag(I) coordination complex [(ina)Ag]NO (ina = isonicotinic acid) is introduced as a multifunctional additive for CNC materials. The complex was synthesized via a simple liquid-assisted grinding approach with full conversion and quantitative yield and incorporated into CNC suspensions under mild conditions. Its addition promotes attractive interparticle interactions, leading to a more cohesive CNC network. Consequently, the resulting cryogels exhibit a more compact morphology and a greater than 2-fold increase in compressive modulus compared to pristine CNC cryogels. In contrast, analogous systems containing AgNO show negligible mechanical improvement, highlighting the importance of the coordination environment. Furthermore, CNC materials containing [(ina)Ag]NO display broad-spectrum antimicrobial activity. These findings establish coordination compounds as multifunctional additives capable of reinforcing CNC materials while introducing non-native functionality.
Biomacromolecules
· 2026 Jun · PMID 42359804
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Alcohols used as cosolvents with water are known to have a broad range of effects on the native triple helix structure of collagen, from its stabilization (e.g., by glycerol) to its denaturation or its fibrillar precipit...Alcohols used as cosolvents with water are known to have a broad range of effects on the native triple helix structure of collagen, from its stabilization (e.g., by glycerol) to its denaturation or its fibrillar precipitation (e.g., by ethanol). We consider gelatin hydrogels as collagenous supramolecular structures and study their resistance to fracture─a localized, stress-induced denaturation process of the collagenous triple-helix cross-links─in an alcoholic environment. Scanning a series of six alcohols, we find that, independently of their contrasted effect on the thermal melting of collagen helices, all of them hinder crack growth. We show that the corresponding increase of fracture energy is attributable to the effect of alcohols on both the and free energies of solvation, i.e., on their trend to favor the of the collagenous triple helix or the of the gelatin network. We find that the latter effect is dominant, all the more that the surface tension of the alcohol is lower. We propose a rationale for this remarkable correlation in the limit of vanishing cosolvent concentrations based on a cavity-filling approach.