Feasible reutilization of Fe3O4/MnO2 Magnetic sorbents were recycle utilized to remove Cu (II) from industrial wastewater. In this paper, The Fe3O4/MnO2 composites structure and interface adsorption mechanism were investigated by chemical affinity, zero potentials combining with XRD, FTIR and TEM. The adsorption, desorption and recycle experiments were explored. The results indicated that Fe3O4/MnO2 composites were nano structure with consisting of two layers with Fe3O4 in the core and amorphous MnO2 on the shell. The adsorption mechanism was that the heavy metals substituting for H of Mn–O–H and forming the structure of Mn–O–Me which meant the metals removal was the process of ion exchange. The sorbent removal efficiency of Cu, were 99.76% respectively. The equilibrium data analysis indicated that the Langmuir model was the most appropriate model to describe the adsorption of on the surface of Fe3O4/MnO2 composites. The kinetics studies showed that the adsorption kinetics of heavy metal ions on the surface of Fe3O4/MnO2 composites was significantly appropriate to pseudo-second-order model. The experiments verified that the Fe3O4/MnO2 sorbent being separated from water by external magnetic field for recycling was feasible for environmentally friendly and efficient remove heavy metal ions.