Piezoelectrics are one of the most important materials used for harvesting energies. Several piezoelectric nanostructures have been used to construct nanogenerators (NGs). Nanofibers made by piezo-polymers, especially polyvinylidene fluoride (PVDF) because of their high flexibility, biocompatibility, and low cost, have shown wonderful growth as the key materials for NGs. Despite these favorable properties, fabricated nanofibrous devices still has low efficiency and many studies have been conducted to characterize and improve the performance of the PVDF nanofibers. Here we tried to fabricate PVDF NG device based on align nanofibers to improve the NGs output, using two different methods rotary collector and applying magnetic field. Characteristics of these structures are evaluated utilizing X-ray diffraction, Fourier transform infrared, differential scanning calorimetry, and scanning electron microscopy. Electrical response of fabricated samples is measured through utilization of an impedance analyzer at room temperature. Results demonstrate that crystalline structure increases in both methods but sample fabricated by rotary collector in magnetic field has more improvement in their outputs. This result shows that in addition to the crystalline structure, nanofibers alignment and arrangement play important roles in piezoelectric properties of sample, as well as NG efficiency. These results teach us to establish engineering design rules for wearable power harvesting devices.