Dual Self‐Assembly of Puerarin and Silk Fibroin into Supramolecular Nanofibrillar Hydrogel for Infected Wound Treatment

The treatment of infected wounds remains a challenging biomedical problem. Some bioactive small‐molecule hydrogelators with unique rigid structures can self‐assemble into supramolecular hydrogels for wound healing. However, they are still suffered from low structural stability and bio‐functionality. Herein, a supramolecular hydrogel antibacterial dressing with a dual nanofibrillar network structure is proposed. A nanofibrillar network created by a small‐molecule hydrogelator, puerarin extracted from the traditional Chinese medicine Pueraria, is interconnected with a secondary macromolecular silk fibroin nanofibrillar network induced by Ga ions via charge‐induced supramolecular self‐assembly. The resulting hydrogel features adequate mechanical strength for sustainable retention at wounds. Good biocompatibility and efficient bacterial inhibition are obtained when the Ga ion concentration is 0.05%. Otherwise, the substantial release of Ga ions and puerarin endows the hydrogel with excellent hemostatic and antioxidative properties. In vivo, evaluation of a mouse‐infected wound model demonstrates that its healing effect outperformed that of a commercially available silver‐containing wound dressing. The experimental group successfully achieves a 100% wound closure rate on day 10. This study sheds new light on the design of nanofibrillar hydrogels based on supramolecular self‐assembly of naturally derived bioactive molecules as well as their clinical use for treating chronic infected wounds. In this work, a supramolecular hydrogel antibacterial dressing with a dual nanofibrillar network structure is fabricated. A nanofibrillar network created by a small‐molecule hydrogelator, puerarin, is interconnected with a secondary macromolecular silk fibroin nanofibrillar network induced by Ga ions. The resulting hydrogel features adequate mechanical strength and excellent hemostatic, antibacterial, and antioxidative properties in a mouse infection model.