Highly Stretchable Vitrimer Nanocomposites With Intrinsic Self‐Healing Capability

ABSTRACT This study presents an innovative and sustainable approach toward developing intrinsically self‐healable and stretchable nanocomposites, aiming to address real‐world challenges while supporting the circular economy. In this work, dynamic transesterification chemistry was incorporated into epoxy using a thiol‐based crosslinker, where intrinsic bond‐exchange interactions significantly contributed to achieving self‐healing in composites via covalent adaptable networks. Additionally, a cost‐effective and eco‐friendly reduced graphene oxide (T‐rGO) derived from waste tyres is employed as a functional nanofiller, introducing a sustainable route to enhance performance. These nanocomposites exhibit excellent self‐healing capabilities, achieving a 97% healing efficiency and 100% shape‐memory properties. The incorporation of T‐rGO significantly enhanced the thermal stability and thermomechanical capabilities of composites, demonstrating a flexural strength of 8.8 MPa and a low activation energy of 51.27 kJ/mol. These composites also exhibit remarkable repeated stretchability, with an elongation of up to 160%. Furthermore, an exceptional 93% enhancement in storage modulus is observed at optimal filler composition compared to the virgin epoxy vitrimer. This study offers valuable insights into the development of smart materials with potential applications in soft robotics, actuators, electronics, and healthcare devices.