Two-step growth technique has bi ell applied to van der Waals epitaxy of C-60 films on H-terminated vicinal Si (1 1 1) substrates to improve the film quality. Formations of the high nucleus density of the single domain with the face centered cubic (FCC) structure have been obtained at the initial stage of the two-step van der Waals epitaxy. The growth of the high-quality C-60 films with the single domain structure has been realized by the two-step growth technique in contrast to the films with the double domain structure obtained by the direct growth. The results strongly indicate that the two-step van der Waals epitaxy would have a great potential to obtain the single domain FCC C-60 films with the high quality under the optimized growth condition.