The harm and treatment of methyl blue (MB) were described, and the necessity for the removal of MB by magnetic nanomaterials was explained. Magnetic Ni-Mg-Co ferrites were prepared by the rapid combustion approach of an active nitrate solution and characterized by X-ray diffraction (XRD), scanning electron microscope (SEM), Fourier transform infrared spectrometer (FTIR), energy dispersive spectroscopy, and vibrating sample magnetometer. Magnetic Ni 0.1 Mg 0.7 Co 0.2 Fe 2 O 4 nanoparticles prepared at 400 C with the saturation magnetization of 19.7 emu g À1 and the average diameter of about 15.2 nm were used to adsorb MB from the aqueous medium. The Brunauer-Emmett-Teller (BET) analysis showed that the specific surface area was 143.17 m 2 g À1 and the average pore size was 9.44 nm. The adsorption mechanism of MB onto magnetic Ni 0.1 Mg 0.7 Co 0.2 Fe 2 O 4 nanoparticles was studied, and the results revealed that the adsorption properties conformed the pseudo-second-order kinetics model due to the square deviation values (R 2 > 0.98), and Temkin model could describe the adsorption state of MB onto Ni 0.1 Mg 0.7 Co 0.2 Fe 2 O 4 nanoparticles, which suggested that the adsorption of MB onto Ni 0.1 Mg 0.7 Co 0.2 Fe 2 O 4 nanoparticles was monolayer-multilayer hybrid chemisorption mechanism. When the pH value exceeded 3, the adsorbance reached large value; while, the adsorbance was 97.6% of the initial adsorption value for seven cycles. The electrochemical impedance spectroscopy and cyclic voltammetry curves of MB adsorbed onto the nanoparticles before and after the adsorption were determined.