Porous metal–organic frameworks (MOF)-based hydrogels have recently attracted wide attention in sensing, catalysis, water treatment, and biomedicine. Yet, limited by challenges of insufficient stability, inordinate metal-ion leakage, and weak wound healing efficacy, the design of MOF-based hydrogel dressings for infected wounds has been rarely explored. Here, we propose a “one-nano MOF-two-functions” strategy to demonstrate the molecular engineering of a chemically stable nano MOF, which acts as both a carrier and a dynamic cross-linker, to fabricate functional composite hydrogels. The active amino groups of the MOF are employed to create dynamic networks with aldehyde-bearing alginate, ensuring excellent compatibility of the MOF with the polymer matrix and imparting effective self-healing properties to the resulting hydrogels. Simultaneously, two active ingredients, Cu nanoparticles (NPs) and curcumin, can be loaded into the nano MOF, achieving synergistic anti-inflammatory and antibacterial effects. Assisted by the mechanical stability and drug co-delivery in an infected full-thickness skin model, the MOF-based hydrogel can reduce the bacterial load on the wound by ∼103 times, and promote collagen deposition and angiogenesis by ∼1.5 and ∼3 times, compared with the control group. The “one-nano MOF-two-functions” design exhibits significant potential for high-performance infected wound dressings.