A series of trial tests were carried out to grow BaTiO3 thin films on SrTiO3 substrates in our newly built laser molecular beam epitaxial system. The phase, crystallographic orientation and crystalline quality of the films were investigated by x-ray diffraction theta/2 theta scan, symmetric and asymmetric rocking curves (omega scans) and phi scan. The interfacial microstructures of the BaTiO3/SrTiO3 and the surface morphology of BaTiO3 films were analyzed by cross-section transmission electron microscopy and atomic force microscopy. Under appropriate growth conditions, epitaxial, single-crystal films with fully c-axis oriented tetragonal structure were obtained. The tetragonality was calculated by using {303} asymmetric rocking curve for a BaTiO3 thin film to be 1.027, which is larger than the bulk value of BaTiO3. The BaTiO3/SrTiO3 interface is very abrupt with no transitional layer and the BaTiO3 film exhibits an atomically smooth surface.