This paper carried out the study on removal of ammonium from aqueous solutions by zeolite derived from electrolytic manganese residue (EMR) via a fusion method. The variables of pH, contact time, EMRZ (EMR-based zeolite) dosage, initial ammonium concentration, and competitive cations and anions on the ammonium uptake capacity were systematically investigated in an attempt to illustrate adsorption performance of EMRZ. The results show that these influence factors had a remarkable impact on the ammonium uptake capacity of EMRZ. Maximum ammonium uptake capacity was achieved at pH value 8.0, EMRZ dosage 0.2 g/100 mL, contact time 100 min, initial ammonium concentration 200 mg/L, and temperature 35°C. Under optimized conditions, ammonium uptake capacity onto EMRZ was up to 27.89 mg/g. The competitive degree of cations in ammonium adsorption process follows the sequence of Na+>K+>Ca2+>Mg2+, and the sequence of anion effect on ammonium removal onto EMRZ is CO32− > Cl− > SO42− > PO43−. The adsorption kinetic was explored and best represented by pseudo-second-order kinetic model. And the adsorption isotherm experimental data had best fitness with the Freundlich and Koble–Corrigan model, suggesting that heterogeneous uptake was the principal mechanism adopted in the process of ammonium adsorption. Moreover, calculation of thermodynamic parameters such as change in free energy (ΔG), enthalpy (ΔH), and entropy (ΔS) was carried out and it was determined to be −15.77∼−14.03 kJ·mol−1, +37.66 kJ·mol−1, and +173.38 J·mol−1·K−1, respectively. These parameters confirmed that ammonium uptake onto EMRZ was an endothermic and spontaneous process. Moreover, no obvious deterioration tendency was observed for the regenerated EMRZ compared with fresh EMRZ. These results indicate that EMRZ has wide application prospects in removing ammonium from wastewater.