Synergistic Strategies in the Design of Dynamic Hydrogels: Lessons From the Hydrogen Bonding in the Nature

Dynamic hydrogels face the challenge of balancing performance robustness with dynamic responsiveness, and traditional strategies often fail to address both. Inspired by the synergistic regulation of structure and function through multiple weak interactions in biological systems, this review examines how synergistic strategies centered on hydrogen bonding can resolve this contradiction. We explore how hydrogen bonds, with their short-range, directional, and reversible properties, form hierarchical synergistic networks with hydrophobic interactions, metal coordination, electrostatic interactions, and dipole interactions. Additionally, we emphasize the role of the solvent environment in coordinated regulation, revealing how ions, organic solvents, and small molecules indirectly modulate interpolymer hydrogen bonds by restructuring the hydrogen bond network of water or directly participating in competitive binding, thus governing the macroscopic performance of gels. Based on these synergistic principles, we describe their applications in realizing hydrogel functions such as high strength and toughness, impact resistance, adhesion, self-healing, actuation, shape memory, and luminescence. Finally, we provide an outlook on emerging frontiers, including data-driven design paradigms based on biological data mining and machine learning, as well as the integration of living cells to construct adaptive life-material hybrid systems for next-generation intelligent soft materials.