Inorganic metal oxides based on reversible reactions have advantages of reacting with CO₂ at high temperature over other sorbents. We presented here that the structure promoted calcium-based sorbent is promising for CO₂ uptake. The sorbents were made by wet chemistry routes, and flame spray pyrolysis in the gas phase. The sorbents were nanostructured particles having specific surface areas as high as 70 m²/g. The CO₂ uptake at various temperatures was determined by thermogravimetric analysis. To study the reversibility of the sorbents, several dozens of carbonation/decarbonation cyclic operations were performed. The sorbents demonstrated stable and reversible behavior and high CO₂ uptake capacity, sustaining the maximum molar conversion at more than 60% even after 100 cycles of operations. Sulfur tolerant sorbents were also identified.