Aerosol-assisted chemical vapor deposition using the β-diketonate precursors Sr(tmhd)2 · 2H2O, Fe(tmhd) 3, and Co(tmhd) 3 was investigated for depositing thin films of the mixed-conducting ceramic SrCoyFe1−yO3−δ onto porous α–Al2O3 substrates. Single-phase SrCoyFe1−yO3−δ perovskite films were obtained at a deposition temperature of 550 °C and pressure of 15 mm Hg, whereas deposition at atmospheric pressure produced mixed-phase films. The Co/Fe elemental ratios in the films reflected those in the precursor solution, but the films were depleted in Sr. Reduced-pressure deposition provided a more uniform film morphology than atmospheric pressure, and led to a supported film which was leak-tight to N2 flow.