Third-order electric susceptibility x(3)of tin-phthalocyanine film deposited on a boro-silicated glass plate coated with rubbing-treated polyimide thin film was measured by a method of THG Maker-fringe technique. In the resonant absorption spectral range, the maximum values of x(3)of aggregated tin-phthalocyanine were 220×10−12esu obtained in the direction perpendicular to the rubbing direction, but the values parallel to the rubbing were 47×10−12esu. The large anisotropy of x(3)was induced by a preferred orientation of tin-phthalocyanine microcrystals when anisotropic substrates were heated at 200°C.