A transmission electron microscopy study of epitaxial C60 and C70 films grown on a GeS (001) surface is presented. The relationship between the orientation of the substrate and the films and structural defects in the films, such as grain boundaries, unknown in bulk C60 and C70 crystals, are studied. Small misalignments of the overlayers with respect to the orientation of the substrate, so-called epitaxial rotations, exist mainly in C70 films, but also sporadically in the C60 overlayers. A simple symmetry model, previously used to predict the rotation of hexagonal overlayers on hexagonal substrates, is numerically tested and applied to the present situation. Some qualitative conclusions concerning the substrate-film interaction are deduced. ©1996 American Institute of Physics.