The development of advanced materials to improve the efficiency of photoelectrochemical (PEC) water splitting paves the way for widespread renewable energy technologies. Efficient photoanodes with strong absorbance in visible light increases the effectiveness of solar energy conversion systems. MoS2 in a two-dimensional semiconductor that has excellent absorption performance in visible light and high catalytic activity, showing considerable potential as an agent of PEC water splitting. In this study, we successfully modulated the MoS2 morphology on indium tin oxide substrate by using the metalorganic chemical vapor deposition method, and applied the PEC application. The PEC photocurrent of the vertically grown MoS2 nanosheet structure significantly increased relative to that of MoS2 nanoparticles because of the efficient transfer of charge carriers and high-density active sites. The enhanced photocurrent was attributed to the efficient charge separation and improved light absorption of the MoS2 nanosheet structure. Meanwhile, the photocurrent property of thick nanosheets decreased because of the limit imposed by the diffusion lengths of carriers. This study proposes a valuable photoelectrode design with suitable nanosheet morphology for efficient PEC water splitting.