Wet adhesion is highly demanded in noninvasive wound closure, tissue repair, and biomedical devices, but it is still a big challenge for developing biosafe and tough wet bioadhesives due to low or even nonadhesion in the wet state for conventional adhesives. Inspired by the wet‐adhesion‐contributing factors of mussel foot proteins, a water‐responsive dry robust tissue adhesive PAGU tape is made with thickness of <0.5 mm through fast UV‐initiated copolymerization of acrylic acid (AA), gelatin (Gel), and hexadecenyl‐1,2‐catechol (UH). The tape shows strong cohesive mechanical properties and strong interfacial adhesion bonds. Upon application onto wet tissue, the adhesive tape can conform to the tissue, quickly dry tissue surface through absorbing surface/interfacial water and then allows formation of interfacial bonding with a high interfacial toughness of ≈818 J m−2. Furthermore, it can be readily detached by treating with aq. urea solution. A highly efficient avenue is provided here for producing conformable, tough, and easy detachable wet bioadhesive tapes.
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