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This article discusses a simple approach for the microwave-assisted synthesis of good quality nanosized calcium titanate crystals doped with trivalent Tm and Yb lanthanide ions. The prepared nanoparticles had a microcube-like structure and a crystallite size of ca. 47 nm. The structure of the nanocrystals was analyzed by X-ray diffraction (XRD) and scanning electron microscopy (SEM), and their spectroscopic behavior was examined at a laser excitation wavelength of 350.7 nm. It was found that doping CaTiO3 nanocrystals with Yb and Tm leads to about 250-fold brighter photoluminescence (PL) emissions in the blue and near-infrared regions than that emitted by pure CaTiO3 nanocrystals. The PL emission was correlated with the structural disorder.