To increase the CO 2 capture capacity of hydrotalcites, the influence of alkali (K, Na) metal carbonate loading of activated supported and unsupported hydrotalcites (HT act ) on their CO 2 capture properties was investigated. The alkali-loaded supported hydrotalcites adsorb at 523 K, depending on the alkali metal (Na or K) and the preparation method, 1.7-2.2 mmol CO 2 g -1 HT which exceeds the capacity of unloaded supported HT (1.3 mmol CO 2 g -1 HT ) and K-loaded unsupported HT (∼0.3 mmol.g -1 ). The key for the increase in capacity in alkali-loaded HT is a close contact at least at a mesoscopic level between HT and alkali metal carbonate. The alkali metal carbonate could be successfully introduced either by impregnation of a K 2 CO 3 solution on assynthesized HT or by leaving residual K (or Na), from the synthesis, in the final material. The latter method is advocated since it omits a washing step after precipitation. The increase in capture capacity for alkali loaded HTs points to a higher concentration of defects (low-coordination oxygen sites) on the surface of the activated alkali loaded HTs compared to the unloaded HT. We propose that the higher concentration of adsorption sites is caused by the presence of Na + /K + on the surface of Mg(Al)O x .