Abstract
The exceptional underwater adhesion and self-healing capabilities of mussels have fascinated researchers for over two decades. Extensive studies have shown that these remarkable properties arise from a series of reversible and dynamic molecular interactions involving mussel foot proteins. Inspired by these molecular interaction strategies, numerous functional materials exhibiting strong underwater adhesion and self-healing performance have been successfully developed. This review systematically explores the nanomechanical mechanisms of mussel-inspired molecular interactions, mainly revealed by direct force measurement techniques such as surface forces apparatus and atomic force microscopy. The development of functional materials, including coacervates, coatings, and hydrogels, with underwater adhesion and self-healing properties, is then summarized. Furthermore, the macroscopic material performances are correlated with the underlying molecular mechanisms, providing valuable insights for the rational design of next-generation mussel-inspired functional materials with enhanced underwater adhesion and self-healing properties.