The C60/C70 thin film crystals have been fabricated on the (001) surface of alkali halide substrates, KC1, KBr, and NaCl, and their structures have been studied. The crystal structure analyses by TEM show that the hexagonal closed packing (hep) with lattice parameters of a=10.0 Å and c=16.3 Å and the face-centered cubic (fee) with a=14.2 Å coexist in the C60 thin film crystals. The C70 thin film crystals show an expanded lattice constant of a=10.5 Å from the view perpendicular to the stacking plane. The ratio of hep to fee is dependent on the kind of the substrates and on the substrate temperatures during the crystal growth. The observed reversible change in the Raman spectrum of the C60 thin films implies a rotational molecular motion in the thin film crystals.