In this work, we improved the electromechanical properties, electrostrictive behavior and energy-harvesting performance of poly(vinylidenefluoridene-hexafluoropropylene) P(VDF-HFP)/zinc oxide (ZnO) composite nanofibers. The main factor in increasing their electromechanical performance and harvesting power based on electrostrictive behavior is an improved coefficient with a modified crystallinity phase and tuning the polarizability of material. These blends were fabricated by using a simple electrospinning method with varied ZnO contents (0, 5, 10, 15 and 20 wt%). The effects of the ZnO nanoparticle size and content on the phase transformation, dielectric permittivity, strain response and vibration energy harvesting were investigated. The characteristics of these structures were evaluated utilizing SEM, EDX, XRD, FT-IR and DMA. The electrical properties of the fabrication samples were examined by LCR meter as a function of the concentration of the ZnO and frequency. The strain response from the electric field was observed by the photonic displacement apparatus and lock-in amplifier along the thickness direction at a low frequency of 1 Hz. Moreover, the energy conversion behavior was determined by an energy-harvesting setup measuring the current induced in the composite nanofibers. The results showed that the ZnO nanoparticles' component effectively achieves a strain response and the energy-harvesting capabilities of these P(VDF-HFP)/ZnO composites nanofibers. The electrostriction coefficient tended to increase with a higher ZnO content and an increasing dielectric constant. The generated current increased with the ZnO content when the external electric field was applied at a vibration of 20 Hz. Consequently, the ZnO nanoparticles dispersed into electrostrictive P(VDF-HFP) nanofibers, which offer a large power density and excellent efficiency of energy harvesting.