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The methods of Mössbauer spectroscopy and X-ray diffraction analysis have been used to study the processes of a solid-phase alloying of the iron alloys with a bcc lattice by nitrogen that occur upon ball-mill mechanical activation in the presence of chromium nitrides. It is shown that a deformation-induced dissolution of chromium nitrides in the matrix of pure iron and in that of the alloys Fe–3Al and Fe–6V results in the formation of the substitutional chromium and interstitial nitrogen bcc solid solutions. An additional alloying of iron with aluminum or vanadium under the deformation dissolution of nitrides leads to the escape of aluminum and vanadium from the matrix and to a decrease in the nitrogen content characteristic of the interstitial solid solution proper due to the strong chemical bonding of alloying elements with nitrogen. The subsequent annealing leads to the decomposition of already formed solid solutions with the formation of aluminum, vanadium, and chromium nitrides of extreme dispersion.