Arsenic contaminated natural water is commonly used as drinking water source in some districts of Asia. To meet the increasingly strict drinking water standards, exploration of efficient arsenic removal methods is highly desired. In this study, hierarchically porous CeO2-ZrO2 nanospheres were synthesized, and their suitability as arsenic sorbents was examined. The CeO2-ZrO2 hollow nanospheres showed an adsorption capacity of 27.1 and 9.2 mg g(-1) for As(V) and As(III), respectively, at an equilibrium arsenic concentration of 0.01 mg L-1 (the standard for drinking water) under neutral conditions, indicating a high arsenic removal performance of the adsorbent at low arsenic concentrations. Such a great arsenic adsorption capacity was attributed to the high surface hydroxyl density and presence of hierarchically porous network in the hollow nanospheres. The analysis of Fourier transformed infrared spectra and X-ray photoelectron spectroscopy demonstrated that the adsorption of arsenic on the CeO2-ZrO2 nanospheres was completed through the formation of a surface complex by substituting hydroxyl with arsenic species. In addition, the CeO2-ZrO2 nanospheres were able to remove over 97% arsenic in real underground water with initial arsenic concentration of 0.376 mg L-1 to meet the guideline limit of arsenic in drinking water regulated by the World Health Organization without any pre-treatment and/or pH adjustment. (C) 2013 Elsevier B.V. All rights reserved.