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Perovskite is attracting considerable interest because of its excellent semiconducting properties and optoelectronic performance. In particular, lead perovskites have been used extensively in photovoltaic, photodetectors, thin-film transistors, and various electronic applications. On the other hand, the elimination of lead is essential because of its strong toxicity. This paper reports the synthesis of lead-free calcium titanate perovskite (CaTiO₃) using a solution-processed combustion method. The chemical and morphological properties of CaTiO₃ were examined as a function of its thickness by scanning electron microscopy, X-ray diffraction (XRD), atomic force microscopy, X-ray photoelectron spectroscopy, and ultraviolet–visible spectrophotometry. The analysis showed that thicker films formed by a cumulative coating result in larger grains and more oxygen vacancies. Furthermore, thickness-dependent hysteresis behaviors were examined by fabricating a metal-CaTiO₃-metal structure. The electrical hysteresis could be controlled over an extremely low voltage operation, as low as 100 mV, by varying the grain size and oxygen vacancies.