This paper examines the feasibility of using electrophoretic deposition for producing thin films of cathode materials based on lanthanum nickel oxides (with the lanthanum nickelate La2NiO4 + δ (LNO) as the predominant phase). We have determined the particle size and zeta potential of nonaqueous suspensions of LNO micro- and nanopowders prepared by solid-state reactions, pyrolysis of liquid precursors, and laser evaporation of a target. Using ultrasonic processing, we have obtained stable LNO nanopowder suspensions in acetylacetone and an isopropanol + acetylacetone mixture, which have zeta potentials of +25 and + 38 mV, respectively. Electrophoretic deposition on a dense model cathode has produced thin bilayer coatings from electrode and electrolyte materials (LNO and Се0.8(Sm0.75Sr0.2Ba0.05)0.2O2–δ), which are of interest for solid oxide fuel cell technology.