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.