Copper ferrocyanide-functionalized magnetic nano-adsorbents were successfully synthesized by electrostatic coating of citric acid coated Fe3O4 nanoparticles with polyethyleneimine, and immobilizing copper and ferrocyanide on the surfaces of polyethyleneimine-coated nanoparticles. Radioactive cesium (Cs) adsorption tests were conducted to investigate the effectiveness of the copper ferrocyanide-functionalized magnetic nano-adsorbents toward the removal of radioactive Cs.