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Herein we report the development of synthetic CaO-based sorbents for enhanced CO 2 capture in calcium looping via a template-assisted synthesis approach, where carbonaceous spheres (CSs) derived from hydrothermal reaction of starch are used as the templates. Cage-like CaO hollow microspheres are successfully synthesized only using urea as the precipitant, and the formation mechanism of this unique hollow microsphere structure is discussed deeply. Moreover, cage-like CaO hollow microspheres possess an initial carbonation conversion of 98.2% and 82.5% under a mild and harsh conditions, respectively. After the 15 cycles, cage-like CaO hollow microspheres still possess a carbonation value of 49.2% and 39.7% under the corresponding conditions, exceeding the reference limestone by 85.7% and 148.1%, respectively. Two kinetic models are used to explore the mechanism of carbonation reaction for cage-like CaO hollow microspheres, which are subsequently proved to be feasible for analysis of chemical-controlled stage and diffusion-controlled stage in the carbonation process. It is found the unique hollow microsphere structure can significantly reduce the activation energy of carbonation reaction according to the kinetic calculation. Furthermore, the energy and raw material consumptions related to the synthesis of cage-like CaO hollow microspheres are analyzed by the life cycle assessment (LCA) method.