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Metal-organic frameworks (MOFs) are porous network compounds that result from the reaction between a transition metal and organic ligands. In this work, cesium ions were removed by the use of a synthesized MOF, zinc benzimidazole benzene dicarboxylic acid [Zn(bim)2(bdc)]n(ZBB) in aqueous solution. Removal of cesium ions occurred with an ion-exchange mechanism. Scanning electron microscopy, X-ray diffraction, Fourier-transform infrared spectroscopy, Brunauer–Emmett–Teller, and thermogravimetric analysis were used to characterize ZBB complex. Bach technique was used for adsorption experiments and the effect of pH, time, temperature, and adsorbent dosage were studied. The study of adsorption isotherms indicated that the sorption process best fits Langmuir isotherm. Radiation studies indicated that this synthesized MOF could be used in medium-active wastewaters treatment. The column experiments were also investigated in order to obtain the dynamic capacity of the adsorption process.