A new candidate for fluoride adsorption from water, amorphous Al2O3 supported on carbon nanotubes (Al2O3/CNTs), is reported in this Letter. The adsorption isotherms show that the best fluoride adsorption of Al2O3/CNTs occurs at a pH range of 5.0-9.0. The adsorption capacity for Al2O3/CNTs is about 13.5 times higher than that of AC-300 carbon, 4 times higher than that of gamma-Al2O3 at equilibrium fluoride concentration of 12 mg/l. The broad range of the pH values and high adsorption capacity of Al2O3/CNTs make it very suitable for potential applications in fluoride removal from water.