Photothermal‐Activated Antibacterial Amyloid‐Polyphenol‐Iron Hydrogels for Synergistic Wound Healing

ABSTRACT The design and development of stimuli‐responsive hydrogels with anti‐inflammatory and antibacterial properties have triggered significant progress in wound healing treatment. Herein, we report a thermally triggered supramolecular hydrogel combining potent antibacterial activity with photothermal functionality. The incorporation of Fe 3+ ions into tannic acid (TA), both bound to lysozyme amyloid fibril (Lys AF) networks, serves a dual role: enabling rapid gelation and conferring efficient photothermal transduction. This dynamic self‐assembly is primarily driven by thermally enhanced metal‐ligand coordination between Fe 3+ and the amyloid‐polyphenol complex (LT), while hydrogen bonding contributes to network stabilization. This mechanism is amplified at elevated temperatures and under optimized concentrations. Notably, the formed amyloid‐polyphenol‐iron (LTFe) hydrogel exhibits exceptional photothermal conversion efficiency (88.56%), robust cycling stability, excellent biocompatibility, and potent antibacterial efficacy against both Gram‐negative ( E. coli ) and Gram‐positive ( S. aureus ) bacteria. In vivo studies confirmed that LTFe eradicated pathogens, suppressed inflammatory cytokines, and accelerated wound regeneration. Overall, our work introduces a versatile strategy for designing high‐efficiency and high‐biocompatibility NIR‐responsive hydrogel systems.