One way to increase the adoption of renewable energy technologies is to develop advanced materials that improve the efficiency of photoelectrochemical (PEC) systems. As a two-dimensional semiconductor, MoS2 exhibits strong absorption in the visible light region and high catalytic activity, making it a promising photoelectrode material for PEC applications. Nevertheless, systematic studies aimed at optimizing its properties remain necessary. In this study, the morphology of MoS2 photoelectrodes for PEC applications was controllably engineered by adjusting the deposition time using a metal-organic chemical vapor deposition process. The PEC photocurrent of vertically grown MoS2 nanosheet structures was markedly higher than that of MoS2 nanoparticles. This enhancement is attributed to (i) efficient charge separation within the nanosheet architecture, (ii) improved light absorption, and (iii) an increase in the density of catalytically active sites. In addition, the photocurrent depends on the nanosheet size, with excessively thick nanosheets exhibiting lower performance due to limited photogenerated carrier diffusion lengths. These results provide a systematic photoelectrode design strategy with an optimized morphology for efficient PEC water splitting.