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With widespread utilization of graphene oxides (GO) in industry, it is ineluctably discharged into environment and has been found to be toxic to cells and animals. Effective techniques and functional materials are necessary for the elimination of GO from wastewater. In this work, the GO was removed by the magnetic Fe3O4/MgAl-layered double hydroxide (MLDH) and its oxide (MLDO) from aqueous solution. The effects of dosage, time and solution pH on the removal capacity of the MLDH and MLDO was carried out in detail through batch experiments. The results showed that the MLDH and MLDO can remove GO from aqueous solution quickly and efficiently. The maximum adsorption capacities were 82.4 mg/g of MLDH and 86.7 mg/g of MLDO. The pseudo-second-order equation was well accorded with the adsorption kinetic data. The isothermal data followed the Langmuir and Freundlich models. The interaction mechanisms of GO were ascribed to the surface complexation and electrostatic attraction by using zeta potential determination and XRD spectra. Moreover, the MLDH and MLDO after adsorbing GO can be separated in 10 s by a magnet. The short adsorption time, excellent removal capacity and extremely fast solid-liquid separation indicated that the MLDH and MLDO were potential magnetic adsorbents to remove the GO nanoparticles in aqueous system.