The highly ordered epitaxial growth of C60 films on rubrene single crystals was demonstrated. The C60 crystals growth commensurate with rubrene (001) surface lattice was confirmed by reflection high energy electron diffraction and X-ray diffraction and grazing incident wide-angle X-ray scattering. Depending on growth conditions, several surface morphologies (rounded, hexagonal, and triangular grains) of C60 grains were observed at the initial growth process. Large grains with layer-by-layer step and terrace structure of C60 were observed at the terrace region of rubrene (001) surface. The growth of high-crystallinity C60 films was achieved at high substrate temperature and slow deposition rate. Long migration length on the substrate which was given by enough substrate temperature enabled the formation of large single crystalline domains.