Magnetic carbon spheres have been successfully prepared by the synchronous carbonation and activationof the 8-quinoliolato Fe(III) complexe with sphere morphology, which has been synthesized bysolovthermal method. The obtained composite possesses relatively even pore diameter of 3.8 nm, highsurface area of 335.59m2/g with 52.67 wt.% Fe3O4 coated, and a saturation magnetization (Ms) of35.27 emu/g. Dye separationperformance of the magnetic carbon spheres is investigated using methyleneorange and methylene blue as modle. The resluts show that the maxium adsorption capacity formethylene orange and methylene blue is 128.70mgg 1 and 151.29mgg 1, respectively, and the processcan rapidly reach adsorption equilibrium within 5 min, which is important for the application of the aspreparedmagnetic carbon spheres.