Self-healing and recyclable polymer materials are being developed through extensive investigations on noncovalent bond interactions. However, they typically exhibit inferior mechanical properties. Therefore, the present study is aimed at synthesizing a polyurethane–urea elastomer with excellent mechanical properties and shape-memory-assisted self-healing behavior. In particular, the introduction of coordination and hydrogen bonds into elastomer leads to the optimal elastomer exhibiting good mechanical properties (strength, 76.37 MPa; elongation at break, 839.10%; toughness, 308.63 MJ m⁻³) owing to the phased energy dissipation mechanism involving various supramolecular interactions. The elastomer also demonstrates shape-memory properties, whereby the shape recovery force that brings damaged surfaces closer and facilitates self-healing. Surprisingly, all specimens exhibite clustering-triggered emission, with cyan fluorescence is observed under ultraviolet light. The strategy reported herein for developing multifunctional materials with good mechanical properties can be leveraged to yield stimulus-responsive polymers and smart seals.

This review mainly focuses on the latest development of high-strength and high-toughness polyurethanes based on supramolecular interactions, and provides a comprehensive analysis of the main types, synthetic strategies, and strengthening mechanisms.