Dibis(ethyleneditho)tetrathiafulvalene (BEDT-TTF) was vacuum-deposited onto KC1 {001} and mica {001}. The molecular orientation in thin films and surface morphology were characterized using transmission electron microscopy (TEM), atomic force microscopy (AFM) and X-ray diffraction (XRD). On the KC1 substrates, BEDT-TTF crystals were oriented epitaxially in the relation of (10–2) [020]BEDT-TTF//(001)[001]KC1± 5° Two types of orientations were found in the films on the mica substrates Coexisting with the orientation found in the films on KC1, (2–21)BEDT-TTF//(001)micawas found in the films formed on the mica substrate. However, the two-dimensional epitaxial relationship was not observed in the BEDT-TTF films formed on the mica surface.