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In this work, we attempted to create surface disorder on CaTiO₃ nanocuboids by NaBH₄ treatment with the aim of enhancing the photocatalytic activity. The samples were systematically investigated by XRD, SEM, TEM, BET, XPS, UV–vis DRS, PL, EIS and photocurrent response. The photocatalytic activity of the samples were evaluated by degrading RhB under irradiation of simulated sunlight, UV and visible light. It is demonstrated that NaBH₄-treated CaTiO₃ samples exhibit an obviously enhanced photocatalytic activity. In particular, the sample treated at 0.1 M NaBH₄ solution has a photocatalytic activity ca. 2.0 times higher than pristine CaTiO₃. This is ascribed to the fact that the created surface disorder facilitates the separation of photogenerated electron-hole pairs, and thus more photogenerated holes are able to participate in the photocatalytic reactions.