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Epitaxially grown (100) three-axis-oriented (Ba0.7Sr0.3)TiO3 thin film on (100) platinum (Pt) coated (100) magnesium oxide (MgO) substrate and (100) three-axis-oriented BaTiO3 thin film with BaZrO3 buffer layer were prepared on an MgO(100) substrate using the chemical solution deposition method. The growth of the film was found to depend on the annealing condition. Transmission electron microscope revealed cube-on-cube epitaxial growth. The thin films exhibited a (100) three-axis-orientation that followed the (100) orientation of the MgO substrate and the (100) orientation of the Pt or BaZrO3 bottom layer, as observed from an X-ray pole figure measurement and the selected area electron diffraction patterns.