The β-cyclodextrin-graft-(maleic anhydride-co-acrylonitrule) copolymer (β-CD-g-(MAH-co-AN)) synthesized through radical polymerization reactions of β-cyclodextrin (β-CD) with maleic anhydride (MAH) and acrylonitrule (AN) in the special monomer proportion, chemically modify with amidoxime groups to obtained the new adsorbent, which was terms as amidoxime-functionalized β-cyclodextrin-graft-(maleic anhydride-co-acrylonitrule) copolymer (β-CD-g-(MAH-co-AO)). Based on the characteristic results of Fourier transform infrared spectra (FTIR), scanning electron microscopy (SEM), X-ray Diffraction (XRD), and thermalgravity analysis (TGA) techniques, the grafted nitrile groups were successfully converted to amidoxime groups by reaction with hydroxylamine. In this report, the influence of different factors such as pH value and ionic strength, solid-liquid ratio, contact time, initial U(VI) concentration, and temperature on adsorption was investigated by a batch adsorption experiment. The adsorption process fitting results show that the adsorption followed the Langmuir isotherm model and the maximum adsorption capacity was 0.747 g/g at pH 4.0. In addition, the regeneration performance was investigated by varying the concentration of eluent, temperature, and contact time. Under the desorption condition of 0.10 M HNO3, the adsorbents can be reused 12 times in the case that the adsorption capacity was not significantly reduced. The functionalized copolymer exhibits high selectivity under circumstance of other co-existing ions is present in the solution.