Biomedical researchers have been attempting to construct a wound dressing with the structure and function of a bionic natural extracellular matrix. This dressing would provide a comfortable environment for wound self-healing. In this study, cellulose-collagen fibrous networks were easily fabricated via the one-pot method using genipin in situ crosslinking collagen hydrolysate in cellulose nanofibrous membranes made by electrospinning cellulose acetate and subsequent deacetylation. The morphology, properties, and successful entrapment of collagen in the cellulose fibrous dressings were validated by scanning electron microscopy, element analysis, Fourier transform infrared spectroscopy, Xray diffraction, water-swelling test, and thermal gravimetric analysis. The functional cellulose nanofiber-based composite membranes exhibited a network structure, good thermal stability, and acceptable water resistance. Human epidermal cells seeded on the composite nanofibrous membranes presented favorable growth, indicating good cytocompatibility and suitability of the dressing to the wound. Therefore, these novel cellulose collagen fibrous networks may have potential use in biomedical applications.