The precursors with NiCO3 · 2Ni(OH)2 · 2H2O, Fe2O3 · nH2O coated alumina microspheres were prepared by the aqueous heterogeneous precipitation using metal salts, ammonium bicarbonate and α-Al2O3 micropowders as the starting materials. Magnetic metal Ni, α-Fe coated alumina, core-shell structural microspheres were successfully obtained by thermal reduction of the precursors at 700 ℃ for 2 h, respectively. Powders of the precursors and the resultant metal (Ni, α-Fe) coated alumina micropowders were characterized by scanning electron microscopy, energy dispersive spectroscopy and X-ray diffraction. The results show that optimized precipitation parameters are concentration of alumina micropowders of 15 g/L, rate of adding reactants of 5 mL/min and pH value of 7.5.And under the optimized conditions, the spherical precursors without aggregations or agglomerations are obtained,then transferred into Ni, α-Fe coated alumina microspheres by thermal reduction. It is possible to adjust metal coating thicknesses and fabricate a multilayer structured metal/ceramics, core-shell mierospherical powder materials.