In order to overcome the difficulty in floor area and cost when the sewage treatment plants need to add follow-up devices for the advanced removal of nitrogen and phosphorus, composite modified zeolites (CMZ) were prepared by loading sodium chloride and quaternary ammonium salt onto the low-cost natural zeolites and the removal efficiency by the modified zeolites under different preparation conditions was studied. The results show that the CMZ not only remove ammonium nitrogen, but also remove the phosphorus and nitrate with a high efficiency and these removal processes do not affect each other. Meanwhile, the adsorption data of ammonium nitrogen, phosphorus and nitrate are fitted well with the pseudo-second dynamics equation. When the dosage of the zeolite in actual sewage is 50 g/L, the effluent of municipal water satisfied the first level B can be improved to level A and the high removal efficiency of ammonium nitrogen ,nitrate and phosphorus are as high as 71.09%, 91.18%, 93.11%, respectively. The adsorbed CMZ can be used repeatedly after regenerated by the single NaCl solution and the regenerated time is short and the regeneration process is easy, which provided a promising application prospect to the utilization of CMZ in the actual sewage treatment.