Both polycrystalline and single-crystal films of iron-substituted strontium titanate, SrðTi 0.65 Fe 0.35 ÞO 3−δ , prepared by pulsed laser deposition, show room-temperature magnetism and Faraday rotation, with the polycrystalline films exhibiting higher saturation magnetization and Faraday rotation. The magnetic properties vary with the oxygen pressure at which the films are grown, showing a maximum at pressures of approximately 4 μ Torr at which the unit-cell volume is largest. The results are discussed in terms of the oxygen stoichiometry and corresponding Fe valence states, the structure and strain state, and the presence of small-volume fractions of metallic Fe in single-crystal films grown at the optimum deposition pressure. Integration of magneto-optical polycrystalline films on an optical-waveguide device demonstrates a nonreciprocal phase shift.