This work presents nanofibrous membranes made of poly(vinylidene fluoride) (PVDF) and poly(2-methacryloyloxyethyl phosphorylcholine-co-methacryloyloxyethyl butylurethane) (PMBU) for promoting the healing of acute and chronic wounds. Membranes were prepared by an electrospinning process, which led to matrixes with a pore size mimicking the extracellular matrix. PMBU greatly improves the hydration of membranes, resulting in very low biofouling by protein or bacteria and enhanced blood compatibility while the cell viability remains close to 100%. This set of properties exhibited by the suitable combination of physical structure and material composition led to applying the zwitterionic nanofibrous membranes as wound-dressing materials for acute and chronic wounds. The results demonstrated that the zwitterionic membrane could compete with commercial dressings in terms of wound-healing kinetics and could outperform them with regard to the quality of new tissue. Histological analyses suggested that inflammation was reduced while proliferative and maturation phases were accelerated, leading to homogeneous re-epithelialization. This study unveils another potential biomedical application of antifouling zwitterionic membranes.