Gamma-alumina (γ-Al 2 O 3 ) is one of the most useful support or additive materials in the preparation of dry sorbent for CO 2 capture from flue gas. However, when the γ-Al 2 O 3 was used in the preparation of dry sorbent, the potassium-based γ-Al 2 O 3 sorbent was deactivated by the forming of by-products like KAl(CO 3 )(OH) 2 during CO 2 sorption. To overcome this problem, a new potassium-based sorbent using alpha-alumina (α-Al 2 O 3 ) as a support was developed in this study. This sorbent showed excellent regeneration properties, as well as high CO 2 capture capacity during multiple CO 2 sorption and regeneration tests at 60°C and 200°C, respectively. These results were due to the formation of KHCO 3 , which could be easily regenerated even at 130°C, during CO 2 sorption without by-products like the KAl(CO 3 )(OH) 2 phase, resulting from the structure effect of alumina. From these results, it is concluded that α-Al 2 O 3 can be used as a support or an additive material to design a regenerable potassium-based sorbent which shows excellent regeneration properties even at 130°C.