Poly (vinylidene fluoride) nanofibers (PVDF NFs) have been extensively used in energy harvesting applications due to their promising piezoresponse characteristics. However, the mechanical properties of the generated fibers are still lacking. Therefore, we are presenting in this work a promising improvement in the elasticity properties of PVDF nanofibrous membrane through thermoplastic polyurethane (TPU) additives. Morphological, physical, and mechanical analyses were performed for membranes developed from different blend ratios. Then, the impact of added weight ratio of TPU on the piezoelectric response of the formed nanofibrous composite membranes was studied. The piezoelectric characteristics were studied through impulse loading testing where the electric voltage had been detected under applied mass weights. Piezoelectric characteristics were investigated further through a pressure mode test the developed nanofibrous composite membranes were found to be mechanically deformed under applied electric potential. This work introduces promising high elastic piezoelectric materials that can be used in a wide variety of applications including energy harvesting, wearable electronics, self-cleaning filters, and motion/vibration sensors.