Highly ordered, single-crystal Fe4N films were prepared on single-crystal SrTiO3 (001) substrates by reactive magnetically enhanced dc triode sputtering. Analytical techniques, including x-ray diffraction, reflectivity, ion channeling, and atomic force microscopy, were used to characterize the structure and morphology of the films. The magnetic properties of the films were measured by magnetic force microscopy and superconducting quantum interference device magnetometry. A technique that utilizes anisotropic magnetoresistance was employed for measurement of the magnetocrystalline anisotropy of the Fe4N films. © 2003 American Institute of Physics.