The crystallinity of cadmium titanate (CdTiO₃) was greatly improved when synthesized under mild reaction conditions, in the presence of chloride. The highly crystalline CdTiO₃ showed much enhanced photodegradation of methyl orange (MO) under simulated sunlight. CdTiO₃ was characterized using X-ray diffraction (XRD), transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS), N₂ adsorption/desorption, photoluminescence (PL), and UV/vis spectrometry. The enhanced photodegradation was attributed to the better charge separation owing to its higher crystallinity.