Mn-MgAl hydrotalcite, surface-enriched with Mn, was prepared by thermal decomposition of MgAl hydrotalcite followed by reconstruction of its structure in the presence of Mn(II) cations and atmospheric CO2 as a guest inorganic anion through contacting the decomposed mass with aqueous Mn(II) nitrate solution. The Mn-MgAl hydrotalcite showed very high catalytic activity, stability, and reusability in the liquid-phase selective oxidation of a wide range of alkylaromatics to their corresponding benzylic ketones, using atmospheric pressure of molecular 02 as a sole oxidant under solvent-free and mild reaction conditions. The catalytic performance of Mn-MgAl hydrotalcite was found to be much higher than that of Mn-containing hydrotalcites prepared by different methods or MgAl hydrotalcite catalysts containing various other transition metals and synthesized through similar procedures. (C) 2007 Published by Elsevier Inc.