Multi‐Crosslinked Hydrogels with Instant Self‐Healing and Tissue Adhesive Properties for Biomedical Applications

Abstract Due to the defects like long gelling time, inferior mechanical properties and weak adhesion, in situ forming hydrogels are still restricted in biomedical applications like viscera rupture and targeted therapy. To address these problems, a new kind of multi‐crosslinked hydrogel (G‐OKG‐DA) consisting of gelatin, oxidized konjac glucomannan (OKG), and dopamine (DA) is proposed in this study. The resulting hybrid hydrogel is endowed with a short gelling time (≈3 min) and injectable capacity. According to the mechanical and adhesive tests, G‐OKG‐DA hydrogel shows a robust tensile strength of 23.94 kPa, as well as a higher adhesive strength (≈150 kPa) than commercial fibrin glue. In addition, an instant self‐healing behavior of G‐OKG‐DA hydrogel can be found, which is attributed to multi‐cross‐linking reactions including Schiff‐based dynamic covalent bonds between OKG and gelatin, oxidative polymerization of DA, and catechol‐mediated chemistry like Michael addition and DA–quinone coupling. Importantly, the multi‐crosslinked hydrogel will not compromise its hemocompatibility and cytocompatibility in vitro, suggesting potential applications in biomedical fields as tissue adhesive and implants.