Results are reported from small angle neutron scattering and Mössbauer spectrometry measurements on nanocrystalline Ni 3 Fe. The nanocrystalline materials were prepared by mechanical attrition and studied in the as-milled state, after annealing at 265°C to relieve internal stress, and after annealing 600°C to prepare a control sample comprising large crystals. The small angle neutron scattering ͑SANS͒ measurements were performed for a range of applied magnetic fields. Small differences were found in how the different samples reached magnetic saturation. From the SANS data obtained at magnetic saturation, we found little difference in the nuclear scattering of the as-milled material and the material annealed at 265°C. Reductions in nuclear scattering and magnetic scattering were observed for the control sample, and this was interpreted as grain growth. The material annealed at 265°C also showed a reduction in magnetic SANS compared to the as-milled material. This was interpreted as an increase in magnetic moments of atoms at the grain boundaries after a low temperature annealing. Both Mössbauer spectroscopy and small angle neutron scattering showed an increase in the grain boundary magnetic moments after the 265°C annealing ͑0.2 and 0.4 B /atom, respectively͒, even though there was little change in the grain boundary atomic density.