Cesium removal from aqueous solutions of radioactive waste streams is a challenge in the field of radioactive waste management; this is due to the small atomic radii of Cs+ metal ions and their high migration ability. So, the development of a withstand system for the removal of Cs+ is crucial. In the current study, the removal of radioactive cesium from aqueous solutions using an RO-TLC membrane was studied. Two modifications were conducted; the first is to enlarge the cesium metal ion radii by interacting with mono- and dibasic acids, namely, stearic acid, tartaric acid, citric acid, and EDTA, and the second is the modification of the RO membrane pore size via reaction with the same acids. The modification was confirmed using SEM, FTIR, and EDX analysis techniques. The Cs+ and K+ rejection capacities and water permeability across the membrane at 1.5 bars were evaluated. Along with using the above-mentioned acids, the Cs+ metal ion retention index (RCs) was also obtained. It was found that employing EDTA as a chelating agent in an amount of 1.5 g/L in conjunction with the variation of feed content since it provided the highest value of RCs ~ 98% when used. Moreover, the elution of Cs+ using water, EDTA, ammonia, and HCl is also investigated. The optimal value of the eluent concentration was (0.25 M) HCl. Finally, Langmuir and Freundlich isotherm models were applied for a better understanding of the sorption process. The results of the present work more closely match the Langmuir isotherm model to determine the dominance of the chemical sorption mechanism.