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The problem of water contamination by long-living cesium and strontium radionuclides is an urgent environmental issue. The development of facile and efficient technologies based on nanostructured adsorbents is a perspective for selective radionuclides removal. In this regard, current work aimed to obtain the nanostructured magnetic zeolite composites with high adsorption performance to cesium and strontium ions. The optimal conditions of hydrothermal synthesis were established based on XRD, SEM-EDX, N2adsorption-desorption, VSM, and batch adsorption experiment data. The role of chemical composition, textural characteristics, and surface morphology was demonstrated. The monolayer ion-exchange mechanism was proposed based on adsorption isotherm modeling. The highest Langmuir adsorption capacity of 229.6 and 105.1 mg/g towards cesium and strontium ions was reached for composite obtained at 90 °C hydrothermal treatment. It was shown that magnetic characteristics of zeolite composites allowing to separate spent adsorbents by a magnet from aqueous solutions.