Hydrogels that are mechanically tough and capable of strong underwater adhesion can lead to a paradigm shift in the design of adhesives for a variety of biomedical applications. We hereby innovatively develop a facile but efficient strategy to prepare
hydrogel adhesives with strong and instant underwater adhesion, on-demand detachment, high toughness, notch-insensitivity, self-healability, low swelling index, and tailorable surface topography. Specifically, a polymerization lyophilization conjugation fabrication method was proposed to introduce
tannic acid (TA) into the covalent network consisting of
polyethylene glycol diacrylate (PEGDA) of substantially high molecular weight. The presence of TA facilitated wet adhesion to various substrates by forming collectively strong noncovalent bonds and offering hydrophobicity to allow water repellence and also provided a reversible cross-link within the binary network to improve the mechanical performance of the
gels. The long-chain PEGDA enhanced the efficacy and stability of TA conjugation and contributed to gel mechanics and adhesion by allowing chain diffusion and entanglement formation. Moreover, PEGDA/TA
hydrogels were demonstrated to be biocompatible and capable of accelerating wound healing in a skin
wound animal model as compared to commercial
tissue adhesives and can be applied for the treatment of both epidermal and intracorporeal
wounds. Our study provides new, critical insight into the design principle of all-in-one
hydrogels with outstanding mechanical and adhesive properties and can potentially enhance the efficacy of
hydrogel adhesives for wound healing.