Graphene oxide nanosheets have attracted multidisciplinary attention due to their unique physicochemical properties. Herein, few-layered graphene oxide nanosheets were synthesized from graphite using a modified Hummers method and were characterized by TEM, AFM, Raman spectroscopy, XPS, FTIR spectroscopy, TG–DTA and acid–base titrations. The prepared few-layered graphene oxide nanosheets were used as adsorbents for the preconcentration of U(VI) ions from large volumes of aqueous solutions as a function of pH, ionic strength and temperature. The sorption of U(VI) ions on the graphene oxide nanosheets was strongly dependent on pH and independent of the ionic strength, indicating that the sorption was mainly dominated by inner-sphere surface complexation rather than by outer-sphere surface complexation or ion exchange. The abundant oxygen-containing functional groups on the surfaces of the graphene oxide nanosheets played an important role in U(VI) sorption. The sorption of U(VI) on graphene oxide nanosheets increased with an increase in temperature and the thermodynamic parameters calculated from the temperature-dependent sorption isotherms suggested that the sorption of U(VI) on graphene oxide nanosheets was an endothermic and spontaneous process. The maximum sorption capacities (Q_max) of U(VI) at pH 5.0 ± 0.1 and T = 20 °C was 97.5 mg g⁻¹, which was much higher than any of the currently reported nanomaterials. The graphene oxide nanosheets may be suitable materials for the removal and preconcentration of U(VI) ions from large volumes of aqueous solutions, for example, U(VI) polluted wastewater, if they can be synthesized in a cost-effective manner on a large scale in the future.