Nanocrystalline metallic iron powder was prepared under either Ar or N2 atmosphere by a vibratory ball mill. The X-ray diffractions (XRD) were used to monitor the structure changes during ball milling. Nanostructure of metallic Fe was further studied by Mssbauer effect. The structure of the electron and magnetism of the interface component in Fe nanocrystals was abviously effected by the milling atmosphere.