Polymer blending is a method to provide nanocomposite nanofibers with improved strength and minimal defects. Chitosan exhibits biocompatibility, biodegradability, antimicrobial activity, and wound healing properties. A combination of gelatin and thermoplastic polyurethane (TPU) blends was explored as a means to improve the morphological deficiencies of chitosan nanofibers and facilitate its electrospinnability. The morphology of the electrospun chitosan, chitosan/gelatin, and chitosan/gelatin/TPU blend nanofibers were characterized using scanning electron microscopy (SEM), while the miscibility and thermal behavior of the blends were determined using differential scanning calorimetry (DSC) and Fourier transform infrared spectroscopy/attenuated total reflectance (FTIR/ATR). The optimum results were achieved in blend with 3 wt% chitosan, 8 wt% gelatin, and 5 wt% TPU, which resulted nanofibers with a mean diameter of 100.6 nm ± 17.831 nm.