Co-BaTiO3 epitaxial films were successfully deposited on (0 0 1) SrTiO3 substrates using the laser molecular beam epitaxy deposition. The growth behaviors were well controlled and monitored in situ by reflection high energy electron diffraction. Both the ex situ characterizations with high resolution transmission electron microscopy and X-ray dispersive analysis revealed that the Co nanocrystals in the face-center cubic structure dispersed well in the single BaTiO3 matrix. Our controllable process might provide an efficient way to engineer Co-BaTiO3 nanocomposite films with desired qualities. (C) 2010 Elsevier B.V. All rights reserved.