An unexplained discrepancy exists between the experimentally measured and theoretically calculated magnetic moments of Mn in α-Fe. In this study, we use density functional theory to suggest that this discrepancy is likely due to the local strain environment of a Mn atom in the Fe structure. The ferromagnetic coupling, found by experiment, was shown to be metastable and could be stabilized by a 2% hydrostatic compressive strain. The effects of Mn concentration, vacancies, and interstitial defects on the magnetic moment of Mn are also discussed. It was found that the ground-state, antiferromagnetic (AFM) coupling of Mn to Fe requires long-range tensile relaxations of the neighboring atoms along ⟨111⟩ which is hindered in the presence of other Mn atoms. Vacancies and Fe interstitial defects stabilize the AFM coupling but are not expected to have a large effect on the average measured magnetic moment.