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BaTiO3 thin films in seven thousands of unit-cell layers have been successfully fabricated on SrTiO3 (001)substrates by laser molecular beam epitaxy. The fine streak patte and the undamping intensity oscillation of reflection high-energy electron diffraction indicate that the BaTiO3 film was layer-by-layer epitaxial growth. The measurements of scanning electron microscopy and atomic force microscopy show that surfaces of the BaTiO3thin film are atomically smooth. The measurements of x-ray diffraction and transmission electron microscopy,as well as selected-area electron diffraction revealthat the BaTiO3 thin film is a c-oriented epitaxial crystalline structure.