Abstract
The integration of high strength, super toughness, damage resistance, body-temperature shape memory, and biosafety into a single skin-mimic material system has been a notable challenge in the realm of material science and biomedical applications. In this study, "Lego-like" polyurethane (PU) was selected to amalgamate multiple properties through the design of multilevel structures. By comprehensively designing the chemical and sequence structures of blocks, coordinating weak/strong hydrogen bonds, and achieving rational microphase separation and crystallization, an elastomer was obtained with an exceptional true tensile strength of 1.42 gigapascal, a high fracture energy of 384.7 ± 18.9 kJ/m(2), and a skin-like nonlinear mechanoresponse. The coordination of crystallization and physical cross-linking also guaranteed excellent body-temperature shape memory properties, which are applicable in 4D printing. Moreover, the obtained elastomer is biosafe and has the potential to promote cell proliferation and DNA repair, which will find wide applications in the biomedical field including minimally invasive surgery.