Increasing food demand has resulted in an ever increasing demand for nitrogen fertilizers. Ammonium is the main constituent of these fertilizers and is a threat to aquatic environments around the world. With a focus on the treatment of drinking water, the scope of this study was to investigate the influence of key parameters on the suitability of granular natural zeolites as adsorbents for ammonium. Sorption experiments were performed in artificial matrices by varying the grain size, contact time, ammonium concentration, pH, content of competing ions, and regeneration solutions used. Additionally, natural matrices and the point of zero charge (pzc) were investigated. With an initial ammonium concentration of 10 mgN/L, the grain size was shown to have no significant effect on the sorption efficiency (97–98%). The experimental data obtained was best described by the Langmuir adsorption model (R² = 0.99). Minor effects on sorption were observed at different pH values and in the presence of competing anions. In addition, the pH_PZC was determined to be between pH 6.24 and pH 6.47. Potassium ions were shown to be better than sodium ions for the regeneration of previously loaded zeolites, potassium is also the main competitor to ammonium sorption. The use of tap, bank filtrate, river, and groundwater matrices decreased the ammonium sorption capacity of granular natural zeolites by up to 8%. Based on our results, granular natural zeolites are promising cost-effective adsorbents for drinking water treatment, especially in threshold and developing countries.