Abstract C 60 and C 70 fullerenes were vacuum deposited onto cleaved surfaces of NaCl and mica. Both C 60 and C 70 formed islands during a first stage of growth, indicative of the Volmer-Weber growth mode. The crystal structure of C 60 films on NaCl was f.c.c. with abundant lamella twinning and stacking faults. The structure of C 70 films on NaCl was also predominantly f.c.c. when the substrate was held above about 370 K. The films on NaCl were polycrystalline. On mica, single-crystal epitaxial films were formed for both C 60 and C 70 with the orientation relationship (111) C60 or C70∥(001) mica.