Polyhydroxyurethanes (PHUs), which are synthesized through the aminolysis of cyclic carbonates, avoid the use of toxic isocyanates compared with traditional polyurethanes (PUs) and have aroused great interest. The large number of hydroxyl groups in the network endows PHUs with unique features, such as recyclable properties and fluorescent properties. To establish the high performance and multifunctionality of PHUs, we designed a molecular structure to fabricate PHUs with mechanical robustness, shape memory properties, fluorescent properties, and recyclable properties. The yielded PHU crosslinked by the quaternary thiol and weak but dense hydrogen bonds (H‐bonds) shows unprecedented high mechanical properties with a tensile Young's modulus of 3.13 GPa, comparable to that of polyimide, a tensile strength of 59.2 MPa at room temperature and an excellent toughness of 27.9 MJ/m3 at 50°C, and good damping properties (tanδ ≥ 0.3, temperature range of 35.2°C). Interestingly, fluorescence caused by the aggregation of carbamate within PHUs allows it to be applied for damage self‐reporting to visualize tiny cracks or magnify fractures. Furthermore, both the thermosetting PHUs and recycled thermosetting PHUs presented excellent shape memory performance. This study provides certain inspiration for the design and development of highly rigid multifunctional polymers.
scite is a Brooklyn-based organization that helps researchers better discover and understand research articles through Smart Citations–citations that display the context of the citation and describe whether the article provides supporting or contrasting evidence. scite is used by students and researchers from around the world and is funded in part by the National Science Foundation and the National Institute on Drug Abuse of the National Institutes of Health.