In this study, nanocomposite scaffolds were developed to regenerate full-thickness skin wounds. New bilayer fibrous constructs were fabricated using polylactic acid (PLA) as the outer layer and gelatin/honey blend (GH) containing different masses of selenium nanoparticles (0 µg, 1 µg, 10 µg, and 40 µg) as the inner layer of wound dressings. Nanocomposite wound dressings were evaluated by SEM, ATR–FTIR, surface wettability, swelling, degradation rate, and mechanical tests. The biocompatibility of nano constructs was evaluated by MTT assay after rat mesenchymal stem cells seeding onto the wound dressings. The full-thickness skin wounds were created on the back of rats, and the nanocomposite fibers were implanted. The PLA/GH/40 µg was a functional wound dressing and accelerated skin regeneration.