Zeolites were synthesized from silica-rich (SF-Z) and calcium-rich (CF-Z) fly ashes, respectively, and their performance in immobilizing ammonium and phosphate was investigated through batch experiments. The cation exchange capacity and phosphate immobilization capacity of SF-Z were identified as 2.79 meq/g and 12.97 mg/g while those of CF-Z were 0.69 meq/g and 87.41 mg/g, respectively. The mixture of SF-Z and CF-Z (MSC-Z) immobilized simultaneously ammonium and phosphate, and the ratio of SF-Z to CF-Z depended on the ammonium and phosphate concentrations in wastewater and the discharge standard. The adsorption processes of ammonium and phosphate on MSC-Z followed Ho's pseudo-second-order model and the intra-particle diffusion was a rate-controlling step. The Langmuir model produced better suitability to the equilibrium data. The thermodynamic study revealed that the adsorption of both ammonium and phosphate on MSC-Z was an endothermic reaction. After treatment by MSC-Z, the ammonium and phosphate concentrations in wastewater from a sewage treatment plant decreased from 7.45 and 1.42 mg/L to 2.06 and 0.51 mg/L, respectively, and met Surface Water Environment Quality Standard in China δ. These results show that the immobilization of ammonium and phosphate in wastewater can be achieved by the combination of zeolites synthesized from silica-rich and calcium-rich fly ashes.