Recent Advances in Self‐Healable Intelligent Materials Enabled by Supramolecular Crosslinking Design

High‐performance intelligent materials with unique stimulus‐responsive properties are highly desired in the future as the rapid development of intelligent systems for Internet‐of‐Things applications. During their long service life, the irregularity in external stimuli and repetitive motions always result in unavoidable permanent damages, where the self‐healing ability inspired by skin is indispensable and highly attractive. However, the introduction of supramolecular networks to achieve self‐healing ability based on reversible dynamic noncovalent bonds usually leads to relatively low strength, while the conflict between high mechanical properties and high self‐healing efficiency is still a great challenge. Moreover, the lack of efficient interfacial interaction between functional layer and self‐healable polymer matrix leads to a permanent function loss during the healing of matrix. Herein, a brief overview of self‐healable sensors and actuators based on recent strategies including multiple noncovalent interactions, covalent–noncovalent interactions, and interfacial supramolecular crosslinking is presented. The advantages and applications of high‐performance self‐healable sensors and actuators enabled by interfacial supramolecular crosslinking are discussed emphatically, and the conclusions and outlooks of self‐healable intelligent materials are presented.