The effect of cyclic carbonation−decarbonation operating parameters on Zr-doped CaO sorbent CO2 uptake capacity evolution is examined. It is revealed that the capacity steady state value increases with the decrease in the carbonation temperature, CO2 concentration in the gas flow upon carbonation and with the increase in the heating rate from the carbonation to the decarbonation stages. The rise in decarbonation temperature leads to a dramatic decrease in the sorbent performance. It is found that if carbonation occurs at 630 °C in the gas flow containing 15 vol.% CO2 and decarbonation is carried out at 742 °C, the sorbent shows the highest values of the initial and steady state CO2 uptake capacity, namely, 10.7 mmol/g and 9.4 mmol/g, respectively.