Vertically aligned WS2 (VAWS(2)) nanosheet films are prepared using a lithium based anodization electrolyte to fabricate WO3 films followed by sulfurization. The VAWS(2) synthesized here is self-organized as a conformal structure to expose active edge sites for water splitting. These vertically aligned nanosheets are composed of exfoliated WS2 to provide abundant active edges for catalytic reactions. Hydrogen evolution activity of the VAWS(2) is demonstrated to show high catalytic current, low onset overpotential and small Tafel slope. By certain measures, this VAWS(2) nanosheet film outperforms some of the state-of-the-art hydrogen evolution reaction (HER) catalysts, which opens up a new pathway to simply and scalably fabricate high-performance water electrolysis catalysts.