Developing effective internal wound dressing materials is important for postoperative tissue regeneration while remains a challenge due to the poor biological environment-adaptability of conventional materials. Here, we report an example of injectable self-healing hydrogel based on gastric environment-adaptive supramolecular assembly, and have explored its application for gastric perforation healing. By leveraging the gastric environment-modulated supramolecular interactions, the self-assembled hydrogel network is orchestrated with sensitive thermo-responsibility, injectability, printability and rapid self-healing capability. The hydrogel dressing can effectively inhibit the attachment of microorganisms and demonstrates outstanding antibiofouling property. In vivo rat model further demonstrates the as-prepared hydrogel dressing simplifies the surgical procedures, reduces postoperative complications as well as enhances the healing process of gastric perforation compared with the conventional treatment. This work provides useful insights into the development of biological environment-adaptive functional materials for various biomedical applications.

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Biological tissues are capable of stiffening and self-healing as they are strained or damaged in order to preserve their integrity and functionalities. However, mimicking both strain-stiffening and selfhealing functions of biological tissues in biocompatible flexible hydrogels remains a challenge. Here, we report a flexible hydrogel constructed by two biocompatible polymers, which can smartly adopt biological strainstiffening or self-healing strategy to maintain the structural integrity and functionalities in response to mechanical deformation. The hydrogel can be reversibly and repeatedly stiffened up to eight times of its original modulus as it is strained, without showing mechanical hysteresis. Besides, the damaged hydrogel can repeatedly self-heal within seconds and fully retains the strain-stiffening capability. In addition, benefitting from the excellent biocompatibility and dynamic nature, the biomimetic hydrogel can be facilely applied for 3D cell encapsulation. This work provides novel insights into the molecular design of tissue-like self-protective soft materials, which may also inspire the development of biomimetic cell culture matrices, artificial tissues, as well as soft machines and robotics for various biomedical and engineering applications.

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Implantable medical devices have been widely applied in diagnostics, therapeutics, organ restoration, and other biomedical areas, but often suffer from dysfunction and infections due to irreversible biofouling. Inspired by the self‐defensive “vine‐thorn” structure of climbing thorny plants, a zwitterion‐conjugated protein is engineered via grafting sulfobetaine methacrylate (SBMA) segments on native bovine serum albumin (BSA) protein molecules for surface coating and antifouling applications in complex biological fluids. Unlike traditional synthetic polymers of which the coating operation requires arduous surface pretreatments, the engineered protein BSA@PSBMA (PolySBMA conjugated BSA) can achieve facile and surface‐independent coating on various substrates through a simple dipping/spraying method. Interfacial molecular force measurements and adsorption tests demonstrate that the substrate‐foulant attraction is significantly suppressed due to strong interfacial hydration and steric repulsion of the bionic structure of BSA@PSBMA, enabling coating surfaces to exhibit superior resistance to biofouling for a broad spectrum of species including proteins, metabolites, cells, and biofluids under various biological conditions. This work provides an innovative paradigm of using native proteins to generate engineered proteins with extraordinary antifouling capability and desired surface properties for bioengineering applications.

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