Atomic ordered Ni 3 Fe single crystals with the L1 2 structure are investigated via X-ray diffraction using synchrotron radiation. A study is performed of the material's structure obtained at room temperature as a result of severe plastic deformation of the single crystals in Bridgman anvils. After compression and subsequent torsion of the samples through different angles, the state atomic ordering changes up to complete disappearance of the L1 2 superstructure, the violation of single crystallinity, and the formation of an ultrafine grained structure.