The precursors for nanosized alpha-Fe- and Al2O3-Fe-coated cenospheres were synthesized by the aqueous heterogeneous precipitation using ferrous (II) sulfate, ammonium bicarbonate, ammonium aluminum sulfate and cenospheres as main raw materials. Subsequently, the composite microspheres with magnetic coatings of alpha-Fe in grain sizes of about 50nm were successfully obtained by reduction of the as-prepared precursors in an H-2/N-2, atmosphere at 720 degrees C for 2 h. The morphology, composition, phases of the precursors and the derived composite microspheres were characterized by scanning electron microscopy (SEM), energy dispersive spectroscopy (EDS), X-ray diffraction (XRD). The magnetic properties of the nanosized alpha-Fe-and Al2O3-Fe-coatcd cenospheres were measured by vibrating sample magnetometer (VSM). On the basis of tests, optimized processing parameters for fabrication of nanosized a-Fe- and Al2O3-Fe-coated cenospheres were determined and the multilayered Al2O3/20 wt.% Fe/cenospheres exhibited very higher coercivity value of approximate 203 Oe compared about 79 Oe of the 20% Fe/cenospheres. (c) 2007 Elsevier B.V. All rights reserved.