Novel magnetic adsorbents with CeO 2 nanoparticles (about 20nm) coated on CuFe 2 O 4 nanofibers were fabricated by combining electrospinning technique and chemical precipitation methods. The prepared CuFe 2 O 4 @CeO 2 composite nanofibers show a diameter of 200nm with a high specific surface area of 64.12m 2 /g. These composite nanofibers exhibit a typical soft-magnetic materials behavior with a specific saturation magnetization (M s ) of 20.51Am 2 /kg. The adsorption performances of these composite nanofibers were evaluated by column bed studies for methyl orange (MO) removal from aqueous solution. The effect of pH, flow rate and dye concentration on adsorption performances were investigated. The results show that the adsorption capacity decreases with increase of pH. The largest adsorption capacity of the column beds shows about 100g/mL under the condition of C 0 =0.05mg/mL, F=2.0mL/min and pH 4.0. The kinetic process is described by Thomas model. The rate constant decreases with the extension of reaction time and decreasing pH. The desorption behaviors are also studied in 0.5M NaCl solution, ethyl alcohol and deionized water, respectively, which show that the adsorbed MO molecules can be easily desorbed from CuFe 2 O 4 @CeO 2 composite nanofibers in NaCl solution. The adsorption mechanism of ionic interaction, formation of hydrogen bonds and pore diffusion is rationally proposed.