Carbon dioxide (CO2) capture is a process that can significantly reduce the amount of CO2 in the atmosphere. In this study, several solid sorbents were examined for their CO2 capturing performance over 30 carbonation–calcination cycles. The sorbents included natural calcined Cadomin limestone (denoted as CD), hydrated calcined Cadomin pellets (denoted as CP), core/shell sorbets with CD and CP as cores, and mesostructured silica (denoted as CD@Si and CP@Si, respectively) and titania (denoted as CD@Ti and CP@Ti) as shells. The core/shell sorbents were prepared with a protective porous shell using the mesoporous silica and titania layers. The surface morphology and porosity of all sorbents were qualified using scanning electron microscopy and were quantified using nitrogen physisorption. X-ray diffraction was also used to identify the crystal phase composition of the sorbents before and after calcination. The CP@Ti pellets showed the best performance in the retention of CO2 uptake over 30 cycles with an activity loss of 50.9%. This is attributed to the formation of a protective layer of thermally stable mesoporous titania using a sol–gel method, which prevented the aggregation of CaO crystals and sorbent sintering. Although the modified core/shell sorbents exhibited an improvement in maintaining the stability of the cyclic operation compared to natural limestone, further study is needed to understand the core/shell sintering phenomenon at high temperatures using other novel materials.