Nanoscale zero-valent iron (NZVI) was first assembled on magnetic carbon/Fe3O4 (CM) with a combination of hydrothermal and liquid phase reduction methods. The novel NZVI@CM magnetic nanocomposites have the merits of large surface area, unique magnetic property, low cost and environmental friendliness. They can be used for Pb(II) removal in aqueous solution. The materials were characterized by using transmission electron microscopy (TEM), X-ray diffraction (XRD), Fourier transform-infrared spectroscopy (FT-IR), thermogravimetric analysis (TGA), vibrating sample magnetometry (VSM), X-ray photoelectron spectroscopy (XPS) and Brunauer–Emmett–Teller (BET) adsorption. The various parameters, such as reaction time, dosage of catalyst, solution pH and acid ions concentrations were studied. The removal efficiency of Pb(II) can be obviously increased by the combination of appropriate CM and NZVI. The removal efficiency of Pb(II) is 99.7% by using 60 mg of NZVI@CM at pH 7. The kinetics study indicates that the Pb(II) removal accords to pseudo-second-order kinetics model.