The degree of crystalline order of evaporated and cast palladium phthalocyanine films was investigated before and after they were submitted to a voltammetric process. X-ray diffraction and UV-vis spectroscopy measurements demonstrated that the electrochemical treatment improves the crystalline quality of the films. The X-ray results revealed an increase of the average size of the crystallites composing the films as well as a decrease in the spacing between the lattice planes in the direction perpendicular to the surface of the film. Optical measurements showed that the electrochemical treatment also introduces an appreciable degree of in-plane ordering. These improvements of crystalline order are observed in both types of films, cast and evaporated, which indicates that the ordering is a direct consequence of the electrochemical treatment and not of the method used for the film deposition. Copyright (c) 2005 Society of Porphyrins & Phthalocyanines.928993