Deposition of La0.6Sr0.4Co0.2Fe0.8O3 (LSCF) oxide films on Gd-doped ceria (CGO) substrates by an electrostatic-assisted ultrasonic spray pyrolysis (EAUSP) method was demonstrated for the first time in this work. The electrostatic field employed for directing the aerosol stream toward the substrate was shown to be indispensable for film deposition. The X-ray diffraction result indicates that a single phase of cubic perovskite was obtained in the calcined films. Scanning electron microscopy examination reveals that the electric field strength had a profound effect on film porosity with weaker field, resulting in higher porosity. The results of impedance measurement on LSCF//CGO//LSCF cells indicate that the area specific resistance values of current LSCF films and their activation energies are comparable to that obtained by conventional sample preparation routes. In view of the simplicity, efficiency, and economy of film deposition, and the sound electrochemical characteristics of the obtained films manifested in current work, it is concluded that the EAUSP method is a promising method for preparation of SOFC electrode films. (c) 2006 The Electrochemical Society.