Room-temperature self-healing waterborne glassy polyurethane via a disordered hydrogen bonding network

In an era driven by carbon neutrality and circular economy imperatives, the development of glassy polymers that intrinsically self-heal at room temperature is highly desirable for energy-efficient and sustainable applications, while these properties typically demand opposing degrees of polymer network mobility. Here, we report a waterborne glassy polyurethane that features a high density of disordered hydrogen bonds, and shows both significant mechanical performance (a Young's modulus of 1.5 GPa and a yield strength of 39.1 MPa) and rapid self-healing ability under ambient conditions. We show that the loosely stacked disordered hydrogen bonds not only permit limited chain mobility in the glassy state but also facilitate the dynamic exchange of complementary moieties, thereby enabling network reconfiguration at room temperature. Furthermore, the material can be readily recycled through dissolution in ethanol without performance degradation, demonstrating its potential as a sustainable polymer platform.