Li2ZrO3 nanocrystals with improved CO2 capture properties were synthesized by a citrate sol-gel method. The morphology and structure of the synthesized Li2ZrO3 samples were characterized in detail by SEM, TEM, and XRD techniques. The CO2 capture-regeneration properties of these nanocrystals were investigated by thermogravimetric analysis (TGA) over a wide range of temperatures and of CO2 partial pressures. The nanosized Li2ZrO3 crystallites with a tetragonal phase exhibit a better CO2 capture performance than reported sorbents, exhibiting a faster uptake and a higher, nearly stoichiometric adsorption capacity (similar to 26 wt.%). Furthermore, the adsorbent shows a good stability, confirmed by capture-regeneration cycles. Based on these excellent properties, application in sorptionenhanced reaction process (SERP) is anticipated.