This study investigated the adsorption properties of graphene oxide in a magnetic-assisted adsorber for the depollution of water containing heavy metals. Two samples of graphene oxide with different surface chemistry were synthetized and assessed using the magnetic-assisted adsorption systems. One graphene oxide sample exhibited a dual magnetic behavior presenting both diamagnetic and ferromagnetic phases, while the other graphene oxide was diamagnetic. The adsorption properties of these graphene oxide samples for removing Pb²⁺ and Cu²⁺ were tested and compared with and without a magnetic field exposure. The results showed that the Pb²⁺ removal increased using both graphene oxide samples in the magnetic-assisted configuration, while Cu²⁺ adsorption was less sensitive to the application of the magnetic field. A monolayer model was used to simulate all the heavy metal adsorption isotherms quantified experimentally. It was concluded that the adsorption mechanism designed to remove Pb²⁺ and Cu²⁺ using tested graphene oxide samples was mainly multi-ionic where two metallic cations could interact with one active site (i.e., oxygenated functional groups) from the adsorbent surface. The oxygenated surface functionalities of graphene oxide samples played a relevant role in determining the impact of magnetic field exposure on the heavy metal removal efficacy. Magnetic-assisted adsorption using graphene oxide is an interesting alternative to reduce the concentration of Pb²⁺ in polluted effluents, and it can also be applied to improve the performance of adsorbents with a limited concentration of oxygenated functional groups, which usually show poor removal of challenging water pollutants such as toxic heavy metals.