The discharging of ammonium from industrial, domestic, and livestock sewage has caused eutrophication of the water environment. The objectives of this study are to synthesize magnetic zeolite (M-Zeo) by an eco-friendly, economical, and easy procedure and to investigate its suitability as an adsorbent to remove ammonium from an aqueous solution. Based on characterization from XRD, BET, and SEM-EDS, Fe3O4 was proved to successfully load on natural zeolite. The effect of pH, temperatures, reacting times, initial ammonium concentrations, and regeneration cycles on ammonium adsorption was examined by batch experiments. The ammonium adsorption process can be best described by the Freundlich isotherm and the maximum adsorptive capacity of 172.41 mg/g was obtained. Kinetic analysis demonstrated that the pseudo-second-order kinetic model gave the best description on the adsorption. The value of pH is a key factor and the maximum adsorption capacity was obtained at pH 8. By using a rapid sodium chloride regeneration method, the regeneration ratio was up to 97.03% after five regeneration cycles, suggesting that M-Zeo can be recycled and magnetically recovered. Thus, the economic-efficient, great ammonium affinity, and excellent regeneration characteristics of M-Zeo had an extensively promising utilization on ammonium treatment from liquid.