As an initial stage of the creation of a new solid material for carbon dioxide capture and storage (CCS), the behaviors of CO2 absorption and desorption were investigated in terms of Li2O-TiO2 compounds. The Li4TiO4 specimen began to absorb CO2 at 250 degrees C with the formation of Li2TiO3 and Li2CO3 phases. The absorption rate was significantly enhanced at 710 degrees C by the formation of the Li2CO3-based liquid phase. Decomposition of Li2TiO3 was observed above 960 degrees C in CO2 atmosphere and above 900 degrees C in Ar-10%CO2 atmosphere. In the formation of solid Li2TiO3 after Li4TiO4/CO2 reaction below 700 degrees C, the reaction rate of CO2 absorption increased with the decreasing diameter of Li4TiO4 particles. The area ratio of the Li4TiO4 phase decreased and that of the Li2TiO3 phase increased in the Li4TiO4 sample after repeating the reaction path of CO2 absorption and desorption.