Dual‐Network Cellulose Adhesives via Copper Coordination: Bridging Ultrahigh Adhesive Performance and Environmental Stability

Abstract High‐performance adhesives play a vital role in both daily life and numerous industrial sectors. Nevertheless, the adhesives currently available on the market generally face several challenges, including insufficient environmental friendliness, limitations in curing conditions, and an imbalance between cost and performance. Herein, a novel and versatile UV curing strategy is developed for the fabrication of dual‐network cellulose adhesives via copper coordination. Strong and tough bio‐based adhesives are prepared by modulating cellulose/adhesive interactions through the compatibility of the natural material of microcrystalline cellulose and copper chloride in methacrylic resin adhesives. The results indicate that the crosslinked network formed by the adhesive passes through the cellulose to the methacrylate resin, further balancing the cohesion and adhesion of the material is achieved with the addition of copper chloride. Notably, the resultant cellulose‐based adhesive displays high strength (32.6 MPa), outstanding shear strength (15.2 MPa), and excellent work of debonding (11 623 N m −1 ), while providing excellent tensile, solvent adaptability, long‐term usability, and closed‐loop recycling performance. This work demonstrates the feasibility of cellulose as a reinforcing agent for conventional adhesives and offers fresh perspectives for exploring bio‐adhesives.