Wounds, particularly under low-hydration conditions, require more time to repair successfully. Therefore, there is an urgent need to develop wound dressings that can accelerate wound healing. Hydrogels, which can maintain a moist environment around the wound and allow gas to pass through the material, act as antibacterial hydrogels as dressings and have great application value in the treatment of wounds. In addition, wound dressings (hydrogels) containing antibacterial capacity have lasting antibacterial effects and reduce damage to cells. In this work, we firstly synthesized two antibacterial agents: imidazolium poly(ionic liquids) containing sulfhydryl (Imidazole-SH) and ε-Poly(lysine) containing SH (EPL-SH). Then, lysine as a cross-linking agent, by “thiol-ene” click reaction, was mixed with Deferoxamine (DFO) to prepare the antibacterial hydrogels. The in vitro assays showed that the hydrogels could effectively kill Escherichia coli (E. coli) and Staphylococcus aureus (S. aureus). In addition, it also could reduce the inflammatory response produced by Lipopolysaccharide (LPS). More importantly, according to the transwell and angiogenesis assays, DFO-incorporated hydrogels promoted the migration and vascular repair of human umbilical vein endothelial cells (HUVECs). All the results revealed that the hydrogels provided new strategies for wound dressings.