Supramolecular chemistry has provided versatile and affordable solutions for the design of intelligent soft materials, but it cannot be applied in stiff materials. This paper describes a new concept for the design of high-performance supramolecular thermosets by using the noncovalent cation-π interaction as cross-linking. These supramolecular thermosets are a class of infusible and insoluble stiff polymers having excellent mechanical properties even at temperatures exceeding 300 °C. The cation-π interaction can be locally and reversibly installed and removed by aqueous treatments at high or low pH, respectively. Local manipulation of cross-linking confers these thermosets with multiple stimuli-responsive functions, such as recyclability, healability, adhesion, and nondestructive detection of cross-linking and mechanical properties.
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