Abstract: Graphene oxide (GO) wrapped Fe₃O₄ nanoparticles (NPs) were prepared by coating the Fe₃O₄ NPs with a SiO₂ layer, and then modifying by amino groups, which interact with the GO nanosheets to form covalent bonding. The SiO₂ coating layer plays a key role in integrating the magnetic nanoparticles with the GO nanosheets. The effect of the amount of SiO₂ on the morphology, structure, adsorption, and regenerability of the composites was studied in detail. An appropriate SiO₂ layer can effectively induce the GO nanosheets to completely wrap the Fe₃O₄ NPs, forming a core-shell Fe₃O₄@SiO₂@GO composite where Fe₃O₄@SiO₂ NPs are firmly encapsulated by GO nanosheets. The optimized Fe₃O₄@SiO₂@GO sample exhibits a high saturated adsorption capacity of 253 mg·g⁻¹ Pb(II) cations from wastewater, and the adsorption process is well fitted by Langmuir adsorption model. Notably, the composite displays excellent regeneration, maintaining a ~90% adsorption capacity for five cycles, while other samples decrease their adsorption capacity rapidly. This work provides a theoretical guidance to improve the regeneration of the GO-based adsorbents.