In the current research, a cost-effective and modified method with a high degree of reproducibility was proposed for the preparation of fine nanoscale and high-purity BaTiO. In contrast to the other established methods, in this research, carbonate-free BaTiO nanopowders were prepared at a lower temperature and in a shorter time span. To reach an in-depth understanding of the scientific basis of the proposed process, an in-detail analysis was carried out for characterization of nanoscale BaTiO particles via differential thermal analysis (DTA)/thermogravimetric analysis (TGA), Fourier transform infrared spectroscopy (FTIR), X-ray diffraction (XRD), scanning electron microscopy (SEM), and transmission electron microscopy (TEM) techniques aided by theoretical calculations. The effects of the temperature and time of calcination process on the preparation mechanism, phase transformation, tetragonality, and particle size of BaTiO were examined. The reaction that results in the formation of barium titanate initiated at approximately 873 K (600 °C) and seemed to be completed at approximately 1073 K (800 °C) and the polymorphic transformation of cubic to tetragonal initiated at approximately 1173 K (900 °C). It seemed to be completed at approximately 1373 K (1100 °C). According to the reaction mechanism, the formation of BaTiO in the initial stage of the interfacial reaction between BaCO and TiO depends on the BaCO decomposition. In the second stage, the BaTiO formation is controlled by barium diffusion through the barium titanate layer. In this stage, in contrast to the literature, no secondary phase was detected. The overall characterizations showed the temperature is more effective than time on the progress in process of preparation because of its diffusion-controlled nature. [ABSTRACT FROM AUTHOR]