The possibility of removing dyes from aqueous solutions containing 137 Cs, 90 Sr, 90 Y, and U(VI) using layered double oxides (LDOs) and hydroxides (LDHs) of Mg and Al was examined. The use of LDO-Mg-Al allows rapid and efficient pretreatment of radioactive solutions containing Cs and Sr radionuclides to remove dyes for the subsequent recovery of Cs and Sr with other selective sorbents. The use of LDO-Mg-Al, LDH-Mg-Al-OH, and LDH-Mg-Al-CD (CD is β-cyclodextrin) allows simultaneous removal from aqueous solutions of UO 2 (NO 3 ) 2 (initial concentration <10 −2 M), 90 Y (an analog of trivalent f elements), and dye (degree of removal >90%).