Crystalline silicotitanate inorganic ion exchanger, with a sitinakite structure is candidate material for remediation of aqueous nuclear waste streams. The syntheses of crystalline silicotitanate (CST) and Nb-substituted crystalline silcotitanate (Nb-CST) were carried out under hydrothermal conditions and the products were characterized using techniques viz., XRD, SEM/EDS, DTA/TGA, surface area respectively. Batch experiments were carried out to study the kinetics of uptake of 137Cs and 90Sr, to estimate the decontamination factor (DF) values and distribution coefficients (Kd) for the above synthesized CST and Nb-CST samples from actual radioactive waste solutions. The DF values for uptake of Cs and Sr by Nb-CST after 24 h of equilibration was 355 and 136 whereas for CST it was found to be 40 and 176 respectively. The Kd values for uptake of Cs and Sr for Nb-CST after 24 h of equilibration was found to be 35,490 and 13,500 mL/g respectively whereas the Kd values for uptake of Cs and Sr for CST was found to be 4,025 and 17,525 mL/g respectively. The ion exchange capacity of Nb-CST towards 90Sr and 137Cs was estimated to be 11.8 and 3.2 meq/g respectively whereas the ion exchange capacity of CST towards 90Sr and 137Cs was estimated to be 14.6 and 4.4 meq/g respectively.