The formation of bulk nanocrystalline alloys based on the Pr60Al 10Ni 10Cu20 bulk metallic glass forming alloy by doping Fe is r eported. B y varying the content of Fe, the microstructure of the Pr-based alloy changes pr ogressively from full glassy state to composite with nanocrystalline particles e mbedded in the glassy matrix, and finally into nano-structured state accompanied by the gradual magnetic property changes. A simple approach to obtain the bulk nanocrystalline material with controllable microstructure is presented, and the relation between microstructure and property is discussed.