Optical absorption spectra (400 similar to 900 nm) of vanadyl phthalocyanine (VOPc) films deposited on perylenetetracarboxylic dianhydride (PTCDA) films formed on mica (VOPc/PTCDA/mica) depended on orientation of polarization plane of incident light. This means that orientations of VOPc and PTCDA molecules in VOPc/PTCDA/mica align. Since the absorption spectrum of the VOPc film with thickness 100 nm in the VOPc/PTCDA/mica formed at 60 degrees C corresponded to that of I-TiOPc, structure of the VOPc film was supposed to be close to I-TiOPc. Without the PTCDA film, orientation aligned II-VOPc film was formed on mica kept at 100 degrees C.