The work aims to prepare ZrO2 films on the surface of zirconium hydride, so as to investigate the effects of Sol pH on hydrogen resistance films. With zirconium n-propoxide as precursor, the sol with pH values of 1, 3, 5, 7 and 9 was obtained by adding hydrochloric acid. The cross-sectional morphologies, surface morphologies and phase composition of the as-prepared ZrO2 coatings were investigated by scanning election microscopy (SEM), confocal laser scanning microscope (CLSM) and X-ray diffraction (XRD), respectively. Hydrogen permeation resistance performance was characterized by vacuum dehydrogenation experiment. The pH of precursor solution had a considerable influence on the film properties and caused difference to the continuity, uniformity and thickness. In contrast, there was no significant change in phase composition, and the ZrO2 films obtained at varied pH mainly consisted of monoclinic phase (m-ZrO2) and tetragonal phase (t-ZrO2) zirconia. The volume fraction of t-ZrO2 and permeation reduction factor (PRF) value of the film exhibited a downward parabolic trend when the pH value was increased from 1 to 9, and the volume fraction of t-ZrO2 and PRF value varied in the range of 13.16% to 46.84% and 10.13 to 19.46, respectively. The pH values of precursor solutions has a considerable effect on the paintability of the sol, thus exerting a direct effects on the quality, phase composition and hydrogen permeation resistance of the ZrO2 films. Particularly, the optimized ZrO2-film coated zirconium hydrides are obtained at the pH value of 3, and the thick films are dense, continuous and uniform, where the max volume fraction of t-ZrO2 and PRF (permeation reduction factor) value are 46.84% and 19.46, respectively.