Single-walled carbon nanotubes (SWCNTs) are functionalized with copper hexacyanoferrate (CuHCF) nanoparticles and therefore constitutes promising solid substrates for the sorption of Cs+ ions from liquid effluents. The high mechanical resistance and large electrical conductivity of SWCNTs are associated to the ability of CuHCF nanoparticles to selectively complex Cs+ ions in order to achieve membrane-like buckypapers presenting high loading capacity of cesium. The materials are thoroughly characterized using electron microscopy, Raman scattering, X-ray photoelectron spectroscopy and thermogravimetric analyses. Cs sorption isotherms are plotted after liquid phase ionic chromatography of the Cs solutions before and after exposure to the materials. It is found that the total sorption capacity of the material reaches 230 mg.g-1, and that one third of the sorbed Cs (80 mg.g-1) is selectively complexed in the CuHCF nanoparticles grafted on SWCNTs. These high values open interesting perspectives in the integration of such materials in electrically driven devices for the controlled sorption and desorption of these ions.