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Nanolamellate structures of CaTiO3 were fabricated by using an in situ hydrothermal synthesis method on titanium for the first time. The number of nanolamellas and the morphology completely or mainly depend on the reaction time and NaOH concentrations, and the wettability of the resulting CaTiO3 surfaces can be successively turned from superhydrophilic to superhydrophobic after modification with a thin layer of hydrophobic silicone, mainly depending on the surface morphology. The proposed formation mechanism of the nanolamellate CaTiO3 structures has also been discussed.