Bioinspired supramolecular polymers with water-triggered dense domains: achieving mechanical robustness, programmability, and weather resistance

Human muscles enhance their mechanical strength through structural training for densification of cellular networks; however, challenges remain in incorporating this feature into synthetic materials. Here, we report a water-triggered supramolecular polymer composed of cellulose and polymethyl methacrylate that achieves over a 22-fold improvement in mechanical properties. During this bioinspired process, water molecules trigger the transition of a stretchable supramolecular network into a densified cross-linked domain. The resultant polymer exhibits a remarkable increase in tensile strength from 2.7 MPa to 61.7 MPa, and demonstrate a substantial flexural strength of 97 MPa, while maintaining impressive structural integrity across a temperature range of -196°C to 180°C. In addition, the polymers possess scalable water-shaping and reinforcement capability, even in seawater or textile wastewater, retaining 100% of their mechanical performance, which allows for customization into tailored geometric structures. Economic analysis and recycling assessment demonstrate that this polymer possesses successful scalability and considerable market. This study provides a biomimetic formulation for the fabrication of high-performance supramolecular polymers, broadening their applications across various fields.