To solve the disadvantages of low adsorption capacity, low utilization and easily desorption of traditional Cu-based adsorbents for radioactive iodide, the inevitable product of nuclear fission, Cu/Palygorskite composite (Cu@PAL) was synthesized through impregnation-reduction method, characterized and applied to remove I^- anions based on the excellent traits of PAL, such as cheap, abundant exchangeable cations and interstratified structure. Results indicate that there are about 7.5wt% copper nanoparticles loaded into PAL for the as-prepared composite. Cu@PAL has better performance in the adsorption of iodide as compared with traditional Cu-based adsorbents, with 72% utilization efficiency and excellent adsorption capacity of 116.1 mg/g. Cu@PAL is suitable for adsorption of I ^- anions under the conditions of neutral, weak acid and the coexistence of interference ions. In addition, the composite exhibit strong oxidation resistance, and the adsorbed product also has strong stability due to the copper stored in the PAL structure.