Here, we report the two-step growth method of two-dimensional (2-D) ZnO nanosheets (NSs) and explore their formation mechanism. Additionally, we illustrate their application for high-performance piezoelectric nanogenerators (NGs) by using grown products from various reaction times. The result shows that NGs based on 2-D NSs demonstrated better output performance than those based on 1-D NWs, which surprisingly increased from ∼40 nA to ∼0.15 μA under the same compressive force of ∼1 kgf. It can also be observed that the output current is slightly elevated as the 2-D nanostructures become thinner. Our results offer a unique way to improve the output performance of NGs by means of controlling the synthesis period of ZnO nanostructures, which have important applications in flexible electronics and wearable devices.