The recovery and recycling of nutrients (N&P) from wastewater are one of the major topics to save primary energy and resources, to raise the efficiency of wastewater treatment plants, and to foster a future circular economy. In the present study, the removal of ammonium (NH ₄ ⁺) and phosphate (PO ₄ ³⁻) using natural and Ca-treated zeolite is investigated in detail. Special emphasis is put on the simultaneous removal of both species from model solutions followed by elaborate mineralogical analyses (XRD, EPMA, FEG-SEM) for zeolite characterization and in order to determine the type, structure, and crystal sizes of CaP-phases precipitating on the zeolites surface. The effectivity of the phosphate segregation and chemical composition and the crystalline structure of the CaP-phase precipitating on the surface of the zeolite depend on the physico chemical conditions in particular on pH, molar ratio of Ca and P (due to zeolite modification), and the presence of NH ₄ ⁺. Results of simultaneous removal experiments of N&P revealed that Ca pretreatment enhances P segregation and increases the obtainable P-loadings of Ca–zeolites. Maximum P-loadings of 25 mg g ⁻¹ Ca–zeolite in binary solutions containing both ammonium and phosphate were obtained. Simultaneous phosphate removal by surface precipitation of CaP-phases does not significantly influence ammonium ion exchange and the type of CaP-precipitates formed on the zeolite surface is assumed to be mainly brushite and apatite.