Microsphere‐Loaded and Borax‐Reinforced Polyacrylic Acid (PAA)/Polyvinyl Alcohol (PVA) Hydrogels Incorporating Tannic Acid: Ultra‐High Toughness and Antibacterial Properties for Artificial Intelligence Skin

Abstract

Hydrogel‐based dressings are widely used in wound healing. Herein, we report a polyacrylic acid (PAA)/polyvinyl alcohol (PVA) composite hydrogel fabricated via self‐catalyzed free radical polymerization, with borax serving as the reinforcing phase. Meanwhile, metal‐ligand coordination bonding between tannic acid (TA) and Fe3+ further elevates the crosslinking density of the hydrogel network. Magnetic chitosan microspheres (MCMs) were synthesized by emulsion cross‐linking and loaded with two antibacterial agents, namely tetracycline hydrochloride (TH) and berberine hydrochloride (Bbh). The incorporation of MCMs into the hydrogel matrix resulted in the development of a multifunctional composite hydrogel suitable for wound dressing applications. Results demonstrated that the composite hydrogel containing a specific concentration of 4‰ (w/v) borax and 20 mg/mL MCMs exhibited superior performance, including enhanced mechanical strength, improved responsiveness, sustained drug release, and potent antibacterial efficacy. The core novelty of this work lies in the synergistic integration of borax‐based mechanical reinforcement, MCM‐mediated dual drug loading and sustained release, and the self‐catalyzed polymerization system. This innovative structural and functional collaboration effectively optimizes the mechanical stability of the hydrogel dressing and achieves synergistic antibacterial and intelligent responsive therapeutic performances, providing a reliable and high‐efficiency candidate for advanced wound care and next‐generation wound dressing applications.