A Spider‐Silk‐Inspired Wet Adhesive with Supercold Tolerance

Abstract Conventional adhesives often encounter interfacial failure in humid conditions due to small droplets of water condensed on surface, but spider silks can capture prey in such environment. Here a robust spider‐silk‐inspired wet adhesive (SA) composed of core–sheath nanostructured fibers with hygroscopic adhesive nanosheath (poly(vinylpyrrolidone)) and supporting nanocore (polyurethane) is reported. The wet adhesion of the SA is achieved by a unique dissolving–wetting–adhering process of core–sheath nanostructured fibers, revealed by in situ observations at macro‐ and microscales. Further, the SA maintains reliable adhesion on wet and cold substrates from 4 to −196 °C and even tolerates splashing, violent shaking, and weight loading in liquid nitrogen (−196 °C), showing promising applicability in cryogenic environments. This study will provide an innovative route to design functional wet adhesives.