Dimensionality plays a vital role at the nanoscale in tuning the electronical and photophysical properties and surface features of perovskite nanocrystals. Here, 3D and 1D all-inorganic CsPbBr3 nanocrystals were chosen as model materials to systemically reveal the dimensionality-dependent effect in photocatalytic H2 evolution. In terms of facilitating photoinduced electron–hole pair separation and charge transfer, as well as inducing proton reduction potential with the presence of fewer Br vacancies, 1D CsPbBr3 nanorods gave about a 5-fold improvement for solar H2 evolution.