Ethylenediaminetetraacetic dianhydride (EDTAD)-modified magnetic-Fe3O4 chitosan (EMC), prepared using the cross-link agent glutaraldehyde and chemicals Fe3O4, chitosan, and EDTAD, was used to compare the adsorption of methylene blue (MB) with magnetic chitosan (MC). The composite structure was confirmed by multiple characterization techniques, including scanning electron microscopy (SEM), X-ray powder diffraction, Fourier transform infrared spectroscopy (FTIR), and potentiometric titration methods. The characterization results suggest that Fe3O4 particles successfully bound on the surface of chitosan, and the EDTAD thoroughly modified the MC. Furthermore, EMC had more amino, carboxyl, and hydroxy groups than typical MC. Adsorption conditions, such as pH values, initial concentrations of MB, reaction temperature, and contact time were systematically examined. In comparison, the maximum adsorption capacity of EMC was approximately twice as much as that of MC. The recovery efficiency for EMC was >80% using 0.1 M HCl as an eluent solution. Therefore, the results reported herein indicate that EMC is very attractive and imply a practical application for dye wastewater treatment.