Mussel‐Inspired and Recyclable Cardanol‐Based Supramolecular Networks for Multifunctional and Sustainable Resins

ABSTRACT Dynamic covalent epoxy resins integrate the merits of thermoplastics and thermosets, enabling reprocessability while maintaining covalent crosslinking. However, achieving simultaneous shape memory, intrinsic flame retardancy, and antibacterial properties in biomass‐derived epoxy resins remains a significant challenge. Inspired by mussel byssus, we developed a supramolecular strategy to construct cardanol‐based epoxy resins incorporating adaptive phosphate networks and robust dynamic noncovalent interactions. The synergistic effects of supramolecular interactions and entropy‐driven dynamics enabled by functional group engineering endowed the material with shape memory ( R f = 99%, R r = 80%), self‐healing, and reprocessability. The conjugated π‐bond system of benzene rings, phenolic hydroxyl radical scavenging, and dynamic phosphate ester carbonization collectively enhanced flame retardancy. The resins achieved a limiting oxygen index of 30.3% and V0 rating under UL‐94 standards. Furthermore, the synergistic antibacterial activity of phenolic polyphenols and phosphate esters resulted in 100% antibacterial efficiency against Staphylococcus aureus . This mussel‐inspired supramolecular design establishes a sustainable platform for next‐generation epoxy resins, offering multifunctional performance critical for medical and food packaging applications under stringent flame retardancy and antibacterial requirements. image