The calcium-based sorbents with a starch pore former and a cement stabilizer were fabricated via the extrusion–spheronization approach for high-temperature CO2capture. The addition of a 10% starch template and 20% cement in the sorbent led to the highest CO2uptake of 0.15 g/g after 20 cycles. With increasing cycle numbers, the gradual decline in CO2-capture capacity was still observed for the modified sorbents. To restore the CO2-capture performance, steam reactivation with various frequencies, steam concentrations, and operational strategies was adopted. After 20 cycles, the CO2uptake stabilized at around 0.41 g/g for the modified sorbent with separate steam hydration after every calcination. The steam introduction during carbonation or calcination recovered the CO2uptake to 0.27 g/g after 20 cycles, which was almost 2 times higher than that of the pellets cycled without steam introduction. Steam hydration reactivation exhibited negative impacts on the mechanical strength of the templated sorbent. The pellets collected after tests with hydration after every 1/3/5 cycles displayed breaking forces less than 1 N, in comparison to the value of 8.82 N for the pellets without hydration. The inferior mechanical strength was attributed to the volume expansion/contraction of pellets during the hydration–dehydration procedure.