Graphene-based aerogels are among the lightest materials in the world and have been extensively studied for environmental remediation. In this work, an FeO/graphene aerogel material was synthesized using the co-precipitation method. The prepared material was characterized using X-ray diffraction (XRD), scanning electron microscopy/X-ray energy dispersive spectroscopy (FESEM/EDX), infrared spectroscopy (FT-IR), and vibration sample magnetization (VSM). The results showed that the FeO nanoparticles with a particle size of less than 100 nm were well-distributed on the surface of the graphene aerogel. The prepared FeO/graphene aerogel showed effective removal of 2,4-D herbicide from the aqueous solution with a maximal adsorption capacity of approximately 42.918 mg g. The adsorption isotherms and kinetics were investigated to study the adsorption behaviour of the resultant material. The saturation magnetism value of the aerogel was determined to be about 20.66 emu g, indicating that the adsorbent could be easily collected from the solution using an external magnet. These results implied that the prepared FeO/graphene aerogel could be a promising adsorbent for the removal of 2,4-D herbicide from water.