Electricity generation using the piezoelectric effect is an important energy harvesting method. In this study, a solar radiation pressure‐driven crater‐shaped light pressure electric generator (LPEG) device with a Pb(Zr0.52, Ti0.48)O3 (PZT) piezoelectric layer and grained Ag layer is fabricated on GaAs(100) wafer. The electrical output of the device is improved by adsorbing Au nanoparticles (AuNPs) on the Ag layer with the surface of closely connected Ag nanoparticles (AgNPs). By controlling the size and concentration of the AuNPs, a maximum power density of 867.5 µW cm−2 is obtained under a solar simulator (AM 1.5G), which represents a 151.7% improvement over the case without AuNP adsorption. The results of Raman spectra, finite‐difference time‐domain (FDTD) simulations, and COMSOL Multiphysics demonstrate that the newly formed hotspots between AgNPs─AuNPs and AuNPs─AuNPs enhance the electric field of the incident light significantly and extend the region where the electric field is maximally amplified to 600–800 nm, resulting in increased solar radiation pressure on the PZT piezoelectric layer.