Extremely strengthening fatigue resistance, elastic restorability and thermodynamic stability of a soft transparent self-healing network based on a dynamic molecular confinement-induced bioinspired nanostructure.

Soft self-healing materials are crucial for the development of next-generation wearable electronics that could function in dynamic environments and resist mechanical damage. However, several challenges remain, including fatigue fracture, poor elasticity, and thermodynamic lability, which significantly limit their practical applications. Here, with a model system of soft self-healing polyurea, we propose a molecular engineering strategy of transforming inherently fragile materials with an island-like structure into resilient ones with a bicontinuous nanophase separation structure using 2-ureido-4-pyrimidinone (UPy) supramolecular motifs as structural regulators. The dynamic and continuous hard domains modified by UPy formed a repairable bicontinuous network similar to those of the reticular layer in animal dermis. This design allows for a simultaneous and tremendous improvement in the fatigue threshold (34.8-fold increase), elastic restorability (the maximum elongation for full dimensional recovery increasing from 6 times to 13 times), and thermodynamic stability (4 orders of magnitude improvement in the characteristic flow transition relaxation time), without significantly compromising the compliance, autonomous self-healing, and optical transparency. These mechanical and thermodynamic improvements address current limitations in unfilled soft self-healing materials as reliable substrates for transparent strain-electronics.