Regulation of Hard Segment Cluster Structures for High‐performance Poly(urethane‐urea) Elastomers

Abstract Elastomers are widely used in daily life; however, the preparation of degradable and recyclable elastomers with high strength, high toughness, and excellent crack resistance remains a challenging task. In this report, a polycaprolactone‐based poly(urethane‐urea) elastomer is presented with excellent mechanical properties by optimizing the arrangement of hard segment clusters. It is found that long alkyl chains of the chain extenders lead to small and evenly distributed hard segment clusters, which is beneficial for improving mechanical properties. Together with the multiple hydrogen bond structure and stress‐induced crystallization, the obtained elastomer exhibits a high strength of 63.3 MPa, an excellent toughness of 431 MJ m −3 and an outstanding fracture energy of 489 kJ m −2 , while maintaining good recyclability and degradability. It is believed that the obtained elastomer holds great promise in various application fields and it contributes to the development of a sustainable society.