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Luminescent perovskite photocatalysts activated by Pr3+ were prepared by combustion. The structural phase, morphology, and chemical composition of the as-prepared photocatalysts were characterized by X-ray diffraction (XRD), scanning electron microscopy (SEM), Brunauer–Emmett–Teller (BET) analysis, and ultraviolet–visible (UV–vis) diffuse reflectance spectroscopy. The photocatalytic activities of the synthesized samples were investigated on the basis of the degradation of methylene blue (MB) under UV light irradiation. CaTiO3:Pr3+ was obtained in high purity and good crystallinity with a perovskite structure. The degradation of the photocatalyst was fitted with pseudo-first-order kinetics according to the Langmuir–Hinshelwood model. Compared to CaTiO3:Pr3+, Ca1–xTiO3:Pr3+ (x = 0–0.3) multifunctional materials exhibit higher luminescence intensity and photocatalytic activity toward the degradation of MB. Ca0.8TiO3:0.1%Pr3+ exhibited the best performance. [ABSTRACT FROM AUTHOR]