Epitaxial ultrathin films of BaTiO3 were prepared using molecular beam epitaxy. For the substrate, (001)-oriented SrTiO3 single crystals were used. Controlling the growth conditions of these films as well as the semiconductor thin films, led to the successful growth of the BaTiO3 films as single crystals, characterized by x-ray diffraction even in the ultrathin range. The ultrathin BaTiO3 films are highly c-axis-oriented tetragonal phaselike bulk BaTiO3 crystals. The tetragonality of the thin film crystals is much larger than bulk crystal’s. We also measured the saturated polarization (Ps) of the BaTiO3 films at temperatures ranging from room temperature to 600 °C. The results confirmed again that the films are ferroelectric tetragonal phase crystals. Moreover, they showed that the transition temperature for the ferroelectric-paraelectric phase transition of the films is higher than bulk crystal’s. © 1998 American Institute of Physics.