This paper reports the role of selection of suitable dielectric layer in nanogenerator (NG) structure and its influence on the output performance. The basic NG structure is a composite material integrating hydrothermally grown vertical piezoelectric zinc oxide (ZnO) nanowires (NWs) into a dielectric matrix. To accomplish this study, three materials - poly methyl methacrylate (PMMA), silicon nitride (Si3N4) and aluminium oxide (Al2O3) are selected, processed and used as matrix dielectric in NGs. Scanning electron microscopy (SEM) analysis shows the well-aligned NWs with a diameter of 200±50 nm and length of 3.5±0.3 μm. This was followed by dielectric material deposition as a matrix material. After fabricating NG devices, the output generated voltage under manual and automatic bending were recorded, observed and analyzed for the selection of the best dielectric material to obtain an optimum output. The maximum peak-to-peak open-circuit voltage output for PMMA, Si3N4 and Al2O3 under manual bending was recorded as approximately 880 mV, 1.2 V and 2.1 V respectively. These preliminary results confirm the predicted effect of using more rigid dielectrics as matrix material for the NGs. The generated voltage is increased by about 70% using Si3N4 or Al2O3, instead of a less rigid material as PMMA.