Herein, a novel composite cathode material of Ni foam supported by amidoxime cellulose microspheres (ACM@Ni) has been prepared. The removal rate of U(VI) can reach 95% within 4 h under the conditions of 298.15 K, pH = 4 and 1.2 V, which was 5 times faster than the physical adsorption. The adsorption data of U(VI) were consistent with the quasi-first-order kinetic and Freundlich isotherm model, revealing the multilayer chemisorption process of uranium on the ACM-5@Ni cathode. In addition, ACM-5@Ni electrode materials also have potential applic...