After the Fukushima accident in 2011, relevant concerns regarding the contamination of the natural environment rose abruptly. For example, water contaminated by radionuclides such as Cs and Sr may directly flow into the ocean and threaten the marine ecosystem. In this respect, costeffective and efficient decontamination techniques need to be developed and verified to remediate the contaminated water. Prussian blue (PB) is known as a representative material that can adsorb Cs by ion-trapping and is widely used for medical purposes. However, there is a limitation that PB itself is non-separable and highly mobile in aqueous system, so it needs a fixture, such as bentonite, to be collected after the adsorption. Furthermore, while the performance of PB toward Cs is relatively well known, its behavior toward Sr has rarely been reported. The object of this study is to investigate the sorption characteristics of Cs and Sr onto PB-functionalized bentonite at various conditions. The adsorbent employed in the present work was prepared by mixing bentonite, FeCl3, and K4[Fe(CN)6] at room temperature for 24 hours in the aqueous solution. The concentrations of FeCl3 and K4[Fe(CN)6] were set to a range of 5-200 % compared to the cation exchange capacity of bentonite. After that, the PB-functionalized bentonite was sieved with a mesh size of 63 μm and then reacted with the Cs and Sr solution at various liquid-to-solid (L/S) ratios of 2-10 g/L for up to 500 minutes. Moreover, synthetic seawater containing additional Cs and Sr was reacted with PBfunctionalized bentonite to characterize the ion selectivity of PB. After the completion of the adsorption experiment, a part of the adsorbent was separated and desorption of Cs and Sr with 2 M of nitric acid was performed. For the quantification of aqueous Cs and Sr concentrations, ICP-MS was employed after the filtration with a pore size of 0.45 μm. The result obtained in this study revealed a high sorption affinity of Cs and Sr onto PBfunctionalized bentonite. The analysis results also presented that the sorption reactions of Cs and Sr reached their steady state within 10 minutes of reaction time. Furthermore, the ion selectivity toward Cs and Sr was verified through sorption test with synthetic seawater. According to the high sorption affinity and selectivity, the PB-functionalized bentonite synthesized through this study is expected to be widely used for remediating the Cs- and Sr-contaminated groundwater and seawater, particularly in nuclear waste-relevant industries.