Unlocking the Power of Multicatalytic Synergistic Transformation: toward Environmentally Adaptable Organohydrogel

Abstract A sustainable and efficient multicatalytic chemical transformation approach is devised for the development of all‐biobased environmentally adaptable polymers and gels with multifunctional properties. The catalytic system, utilizing Lignin aluminum nanoparticles (AlNPs)‐aluminum ions (Al³⁺), synergistically combines multiple catalytic cycles to create robust, mechanically stable, and versatile organohydrogels. Single catalytic cycles alone fail to achieve desired results, highlighting the importance of cooperatively combining different cycles for successful outcomes. The transformation involves free radical crosslinking, reversible quinone‐catechol reactions, and an autocatalytic mechanism, resulting in a dual crosslinking strategy that incorporates both covalent and ionic crosslinking. This approach creates a dynamic gel system with combined energy dissipation and storage mechanisms. The engineered organohydrogels demonstrate vital multifunctionalities such as good thermal stability, self‐healing, and adhesive properties, flame‐retardancy, mechanical resilience and durability, conductivity, viscoelastic properties, environmental adaptability, and resistance to extreme conditions such as freezing and drying. The developed catalytic technology and resulting gels hold significant potential for applications in flexible electronics, energy storage, actuators, and sensors.