Electrospinning has been used to fabricate nanofibrous scaffolds from a variety of synthetic and natural materials, including polyvinyl alcohol (PVA) and gelatin. Although PVA possesses appealing mechanical properties for tissue engineering applications, it lacks adequate cellular recognition sites, which limits the material's bioactivity. In contrast, gelatin has desirable bioactivity but lacks adequate mechanical properties and can be difficult to handle. Therefore, coaxial electrospinning is employed to create nanofibers of these materials in a core/shell structure with gelatin forming the shell and PVA forming the core of the fibers. In this study, scanning electron microscopy (SEM), transmission electron microscopy (TEM), Fourier transform infrared spectroscopy (FTIR), mechanical testing, and cellular studies were utilized to evaluate the morphology and material properties of coaxially electrospun PVA/gelatin nanocomposite scaffolds in comparison to scaffolds composed of solely PVA or gelatin. This study yields insight into the potential of combining synthetic and natural polymers together in the engineering of composite nanofibers for a variety of tissue engineering applications.