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The present work reports on the new approach to create metal-supported Sr2FeMoO6(SFMO)-based electrodes that have high potential to be applied in solid oxide fuel cells. The SFMO films were formed on stainless steel substrates by electrophoretic deposition (EPD) method. Ethyl alcohol with phosphate ester as a dispersant and isopropyl alcohol with I2-acetone mixture as a charge additive were considered as an effective medium for EPD of SFMO particles. The synthesis of SFMO powder as well as suspension preparation and deposition kinetics were systematically studied. The effect of applied voltage on the thickness and morphology of SFMO films was established. The microstructure of the deposits was examined by electron microscopy. The thickness, morphology and porosity of the SFMO layers can be fine-tuned by varying solvent, charging additives, deposition time, and applied voltage. According to X-ray photoelectron spectroscopy analysis, it was found that Fe3+–Mo5+and Fe2+–Mo6+pairs coexist, whereas the valent balance shifts toward an Fe2+–Mo6+configuration.