Supramolecular polymers are usually thermomechanically unstable, as their mechanical strength decreases drastically upon heating, which is a fatal shortcoming for their application. Herein, inspired by heat shock proteins (HSPs) which enable living organisms to tolerate lethal high temperatures, we design an HSP-like response to impart a supramolecular elastomer with high thermomechanical stability. The HSP-like response relies on the reversible hydrolysis of boronic acid and the tunable association strength of boron dative bonds. As the temperature increases, the boronic acid dehydrates and transforms into boroxane. The boroxane, acting as a heat shock chemical, prevents the disintegration of the supramolecular network through formation of multiple and stronger dative bonds with imidazole-containing polymers, thereby enabling the material to retain its mechanical strength at high temperatures. Such chemical transformation and network change induced by the HSP-like response are fully reversible during the heating and cooling processes. Moreover, due to the dynamic nature of the supramolecular network, the elastomer possesses recycling and self-healing abilities.