MoSx as a promising electrocatalyst for hydrogen evolution reaction (HER) has the active sites of rims and edges and inert sites of basal plane. A strategy to activate MoSx is to produce more unsaturated S or S vacancies on the inert plane by designing unique nanostructure. Herein, we report a facile electrodeposition assisted by liquid crystal template (LCT) to prepare MoSx film on ITO substrate (MoSx (LCT)). XPS confirms the state of Mo and S of the obtained MoSx film. SEM shows that there are many uniform disk bulges with the diameter of about 100 nm on the surface of MoSx (LCT), which may provide more rims and edges of MoSx. While the electrodeposited MoSx film in water (MoSx (H2O)) is a smooth plane structure. The electrochemical measurements show MoSx (LCT) exhibits an ultrahigh activity for HER with the small onsetpotential very close to that of Pt/C, which may be due to not only the uniform disk bulges but also the more unsaturated S atoms of MoSx (LCT). The electrodeposition assisted by LCT may be a novel strategy to prepare novel nano structure and activate MoSx-based electrocatalysts for HER. (C) 2017 Hydrogen Energy Publications LLC. Published by Elsevier Ltd. All rights reserved.