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LDHs of Mg and Al, containing CО32– ions in the interlayer space (LDH-Mg-Al-CО3), and layered double oxides of Mg and Al (LDO-Mg-Al) were prepared using MWR. The use of MWR allows not only acceleration of the synthesis of both LDH and LDO, but also preparation of compounds with high kinetic characteristics of the U(VI) sorption. The degree of U(VI) sorption (α) from 10–2 mol/l aqueous U(VI) solutions at a sorption time of 4 h and V/m = 50 ml/g exceeds 99.0%. In sorption from more concentrated (10–1 mol/l) aqueous U(VI) solutions under similar conditions, α on all the samples does not exceed 37.5%. It was found that the use of MWR in the synthesis of LDHMg-Al-CО3 and LDO-Mg-Al allows not only acceleration of the synthesis of both LDH and LDO, but also preparation of compounds with high kinetic characteristics of the U(VI) sorption.