Engineering of Multi‐Dynamic Bonds Toward Room‐Temperature Self‐Healing Epoxy/MXene Adaptable Network with Record‐High Toughness

Abstract Epoxy thermosets with exceptional toughness and self‐healing properties are essential for high‐end manufacturing applications and sustainable development. Conventional epoxy‐crosslinked networks are inherently brittle, leading to a lack of these traits. Drawing inspiration from mussel nacre and byssus, a bionic epoxy/MXene network is developed, featuring a multi‐type dynamic bond system and an inverse‐artificial nacre structure. Through hierarchical assembly, the network integrates side‐chain quadruple hydrogen bonds (H‐bonds), dynamic disulfide bonds, and interfacial H‐bonds, facilitating rapid energy dissipation. This epoxy demonstrates exceptional performance through meticulous engineering, exhibiting impressive toughness (210.75 MJ m −3 ), exceeding that of spider silk by 30%. It also shows remarkable stretchability (864.72%) and rapid self‐healing capabilities (90.0% recovery within 2 h at 25 °C). This combination of these properties is consistently maintained under various environmental conditions due to the protection of the dynamic bonds by the hydrophobic chains. Furthermore, the bionic network enhanced the composites with superior gas impermeability and high interfacial adhesive strength (9.58 MPa). This study offers novel insights into the development of high‐performance, durable protective coatings, and flexible devices designed for enhanced tolerance to harsh marine environments.