Tunable Mechanical, Antibacterial, and Cytocompatible Hydrogels Based on a Functionalized Dual Network of Metal Coordination Bonds and Covalent Crosslinking

Tissue engineering has become a rapidly developing field of research because of the increased demand from regenerative medicine, and hydrogels are a promising tissue engineering scaffold because of their three-dimensional structures. In this study, we constructed novel hydrogels of gelatin methacrylate (GelMA) hydrogels modified with histidine and Zn²⁺ (GelMA-His-Zn(II)), which possessed fascinating antibacterial properties and tunable mechanical properties because of the formation of a functionalized dual network of covalent crosslinking and metal coordination bonds. The introduction of metal coordination bonds not only improves the strength of the GelMA hydrogels with covalent crosslinking but also makes their mechanical properties tunable via adjustments to the concentration of Zn²⁺. The synergistic effect of Zn²⁺ and the imidazole groups gives the GelMA-His-Zn(II) hydrogels fascinating antibacterial properties (up to 100% inhibition). Counting the colony forming units and compression tests confirmed the fascinating antibacterial abilities and tunable mechanical properties, respectively, of the GelMA-His-Zn(II) hydrogels. In addition, Cell Counting Kit-8 assays, cytoskeletal staining assays, and live/dead assays confirmed the excellent cytocompatibility of the GelMA-His-Zn(II) hydrogels. Therefore, the GelMA-His-Zn(II) hydrogels are promising for applications in tissue engineering.