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Thermoset elastomers have been extensively applied in many fields because of their excellent mechanical strengths and durable characteristics, such as an excellent chemical resistance. However, in the context of environmental issues, the nonrecyclability of thermosets has become a major barrier to the further development of these materials. Here, a well-tailored strategy is reported to solve this problem by introducing mismatched supramolecular interactions (MMSIs) into a covalently cross-linked poly(urethane-urea) network with dynamic acylsemicarbazide moieties. The MMSIs significantly strengthen and toughen the thermoset elastomer by effectively dissipating energy and resisting external stress. In addition, the elastomer recycling efficiency is improved 2.7-fold due to the superior reversibility of the MMSIs. The optimized thermoset elastomer features outstanding characteristics, including an ultrahigh tensile strength (110.8 MPa), an unprecedented tensile toughness (1245.2 MJ m
Wang et al. (2024) studied this question.