Copper ions were first adsorbed by zeolite 4A synthesized from bauxite tailings, the desorption of Cu(II) using Na2EDTA solutions was performed, and the recycling of zeolite 4A in adsorption and desorption was systematically investigated. It was observed that the Cu(II) removal efficiency was directly dependent on the initial pH value. The maximum removal efficiency of Cu(II) was 96.2% with zeolite 4A when the initial pH value was 5.0. Cu(II) was completely absorbed in the first 30 min. It was also observed that the desorption efficiency and zeolite recovery were highly dependent on the initial pH and concentration of Na2EDTA in the solution. The desorption efficiency and percent of zeolite recovered were 73.6 and 85.9%, respectively, when the Na2EDTA solution concentration was 0.05 mol L?1 and the pH value was 8. The recovered zeolites were pure single phase and highly crystalline. After 3 cycles, the removal efficiency of Cu(II) was as high as 78.9%, and the zeolite recovery was 46.9%, indicating that the recovered zeolites have good adsorption capacity and can repeatedly absorb Cu(II).