Metallophthalocyanines (MPc’s) have sufficiently large Raman cross sections to obtain high SIN spectra when excited by a 691-nm laser. Both theory and experiment indicate that partial orientation of MPc molecules at solid/gas or solid/liquid interfaces yields depolarization ratios which are quite different from those in solution. For MPc monolayers adsorbed on graphite, the observed depolarization ratios lead to the conclusion that MPc (M = Co, Fe(II), Zn, Mg) molecules are uniaxially oriented upon adsorption with their molecular plane parallel to the graphite basal plane. The results also allow unambiguous assignment of MPc Raman mode symmetry.