The traditional development of CaO-based sorbents to be used in calcium looping process (CLP) consists of two steps: producing powders with improved cyclic performance by sorbent modification, followed by the subsequent granulation. However, this traditional routine is complicated and energy -consuming. Moreover, the improved performance would be weakened again during the granulation process. Hence, the implement of the modification and granulation within one step to produce CaO-based sorbents is of significant importance for CLP. This work, for the first time, proposes a simple and facile gel-casting technique to achieve the one-step synthesis of highly-efficient CaO-based sorbents pellets. The pellets modified with microcrystalline cellulose (CaO-MC) achieved considerable CO2 capture capacity of similar to 0.48 g CO2/g sorbent at the 25th cycle under the mild calcination condition and retained relatively excellent performance of 0.41 g/g over 25 moderate cyclic tests, higher than those of the unmodified pellets (CaO-pellet). The decomposition of microcrystalline cellulose in CaO-MC does not change the cubic crystal structure of CaO, but brings more pores that contribute a lot to its superior CO2 capture performance. Moreover, all synthesized pellets possess good attrition resistance, indicating the applicability of the prepared pellets to the application in CLP. (C) 2017 Elsevier B.V. All rights reserved.