Poly(vinylidene fluoride) (PVDF) nanofibers have tremendous potential in nano-sensing and energy scavenging applications. In this study, uniaxially aligned nanofibers were developed from halloysite nanotubes (HNT)/PVDF nanocomposite using electrospinning technique. Incorporation of HNT into PVDF not only reduced the diameter of the electrospun nanofibers, but, also improved their morphology. Fourier transform infrared spectroscopy, wide angle X-ray diffraction and differential scanning calorimetry techniques were used to characterize the crystallinity, polymorphism and polymer-filler interaction in the nanocomposite nanofibers. A force sensor was indigenously designed to study the piezoelectric responses of the nanocomposite nanofibers. At 10 wt% of HNT loading, the sensor produced the highest voltage output, which can be ascribed to its highest beta-phase content. Incorporation of HNT and use of electrospinning synergistically enhanced the beta-phase content and hence the piezoelectric behavior of PVDF. Hence, these nanofibers could be promising and prominent materials in sensor and actuator applications.