A new cell-loading strategy is proposed to improve the self-healing properties of hydrogels prepared by free-radical polymerization. The introduction of normal human dermal fibroblast (NHDF) cells enables the formation of dually crosslinked hydrogels through hydrogen interactions between cell secretions (mainly the secretory proteins) and polymer chains. This allows an enhancement of the self-healing efficiency from 73% to 92% and an acceleration of the self-healing rate (12 times). Based on the excellent biocompatibility, antibacterial property and low toxicity, we extended the use of dually crosslinked hydrogels as wound dressings to expedite wound healing. This cell-loading concept for constructing dually crosslinked hydrogels offers an available pathway to design smart materials useful for biomedical applications.