In this work, sorbent pellets were prepared based on six synthetic powdery sorbents. CO2 uptake tests and kinetic analysis were carried out to screen sorbent pellets. Experimental results showed that the CO2 capture capacity of sorbent pellets was lower than that of powdery sorbents, which was mainly attributed to reduced Brunauer-Emmett-Teller (BET) specific surface area caused by pore structure damage during the pelletization process. However, the sorbent pellet CaSi75p containing 75 wt % CaO and 25 wt % Ca2SiO4 was less affected by pelletization than other sorbent pellets, which can be explained by the formation of cracks and pores that resulted from the crystalline change of Ca2SiO4 during the calcination-carbonation cycles. Among all of the sorbent pellets, CaSi75p showed the highest CO2 capture capacities of 0.531 g/g and 0.26 g/g in the first and 25th cycles. The performance of sorbent pellets was improved by adding cellulose as a pore-forming material. The reaction rate constants for all sorbents in each cycle were calculated. The experimental and kinetic data indicated that CaSi75p was an excellent sorbent even without adding cellulose.