In this work, we propose an easy, cost-effective, and efficient approach to wrap zinc sulfide (ZnS) nanostructures or other similar nanomaterials with graphene oxide (GO) nanosheets for energy harvesting. The ZnS nanoplates were wrapped with different concentrations of GO nanosheets (5,10,15,20,and 25 wt %) by using the hydrothermal method. Field-emission scanning electron microscopy and powder X-ray diffraction were performed to study the surface morphology and crystal phase structure of each sample. The dielectric study revealed that the wrapping gradually enhanced the polarization density of ZnS nanostructures. Then, GOx-ZnS nanostructures were loaded in a polydimethylsiloxane (PDMS) polymer matrix (GOx-ZnS@PDMS) to develop flexible piezoelectric nanogenerator (FPENG) devices.