Thin films of NiFe2O4 were deposited on SrTiO3 (001) and Y0.15Zr0.85O2 (yttria-stabilized zirconia) (001) and (011) substrates by 90°-off-axis sputtering. Ion channeling, x-ray diffraction, and transmission electron microscopy studies reveal that films grown at 600 °C consist of ∼300 Å diameter grains separated by thin regions of highly defective or amorphous material. The development of this microstructure is attributed to the presence of rotated or displaced crystallographic domains and is comparable to that observed in other materials grown on mismatched substrates (e.g., GaAs/Si or Ba2YCu3O7/MgO). Postdeposition annealing at 1000 °C yields films that are essentially single crystal. The magnetic properties of the films are strongly affected by the structural changes; unannealed films are not magnetically saturated even in an applied field of 55 kOe, while the annealed films have properties comparable to those of bulk, single crystal NiFe2O4. Homoepitaxial films grown at 400 °C also are essentially single crystal.