In this study, ZnO nanosheet structures and copper oxide/ZnO heterojunctions were prepared by means of a cost-effective, low-toxicity, and easier synthesize experimental process was used to fabricate high-density, high-surface-area by atmospheric pressure plasma process-assisted chemical vapor deposition for the application of photoelectrochemical hydrogen generation. The highest solar-tohydrogen conversion efficiency of the ZnO nanosheet structure was 0.01% at 0.6 V(vs. RHE), respectively. To improve the efficiency of photoelectrochemical hydrogen generation of ZnO nanosheets, copper oxide nanoparticles was decorated by the surface of ZnO nanosheets to form a NP junctions to improve the photoelectrochemical hydrogen generation performance. The highest solar-to-hydrogen conversion efficiency of the copper oxide/ZnO heterojunctions was 0.21% at 0.6 V (vs. RHE), which were 21 times more than ZnO.