Mechanical alloying of crystalline, elemental iron and zirconium powder has been performed in a powder ball mill. The amorphicity of the powder has been shown to be in the range 30–78 at.% Fe by X-ray diffraction and thermal analysis. The wavenumbers Q p as a measure for the mean nearest neighbour distance are in good agreement with those for melt-spun or sputtered amorphous FeZr alloys. A detailed investigation of the iron-rich two-phase region by X-ray diffraction and Mössbauer spectroscopy reveals an enhanced primary solubility of 5 at.% Zr in iron. Preliminary crystallization investigation shows that mechanically alloyed Fe 80Zr 20 transforms to Fe 2Zr and α-Fe at 690°C. Further annealing leads to the formation of Fe 3Zr.