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Calcium titanate (CaTiO3) with prism-like-shaped and CaTi2O4(OH)2 nanosheet-like morphology were synthesized by a simple solvothermal route without any surfactants. X-ray diffraction (XRD), field emission scanning electron microscopy (FESEM) and Fourier transform infrared spectroscopy (FT-IR) were employed to investigate the microstructure of the samples. The experimental results showed that NaOH concentration played a key role for the formation of CaTiO3 prisms. With increasing NaOH concentrations, the obtained sample changed from CaTi2O5 aggregated particles to CaTi2O4(OH)2 nanosheets, and then to CaTiO3 prisms. When NaOH concentration was 7 M, CaTiO3 morphology is mainly composed of regular prisms. A rational mechanism was proposed to illustrate the morphology evolution of the samples synthesized at various NaOH concentrations. And the CaTi2O4(OH)2 interlaminar structure was illustrated. [ABSTRACT FROM AUTHOR]