AbstractThe design and fabrication of novel soft bioelectronic materials for rapid wound healing and real‐time monitoring are critical for smart healthcare. However, developing such integrated multifunctional materials devices remains challenging due to fabrication dynamics and sensing interface issues. Herein, a novel strategy is presented for accelerating the kinetics of hydrogels integrating antimicrobial, electrotherapeutic, and wound monitoring functions via bimetallic phenolic networks. The Al3+ catalyzes the radical copolymerization reaction of acrylic acid, resulting in the gelation of the system within 10 s, and also catalyzes the redox reaction between silver and lignin, inducing the sustained release of catechol, which significantly enhances the hydrogel's antimicrobial activity and shortened the wound healing process. Meanwhile, the abundant non‐covalent interactions enhance the hydrogel's tissue adhesion, and mechanical properties (tensile strength 1.558 MPa and elongation 1563%). In addition, the bimetallic ions endow the hydrogels with excellent sensing properties. Under the synergy of electrical stimulation, the wound healing rate is accelerated. Notably, wound assessment can be performed by monitoring changes in electrical signals over the wound, which can assist physicians and patients in achieving intelligent wound management. This work provides new insights into the design and application of multifunctional smart bioelectronic materials.