Abstract Dolomite, a naturally occurring Ca-based sorbent, shows superior recycling stability in carbonation/calcination cycles for CO2 capture. However, the separation between Ca and Mg in sorbent during recycling weakens the resistance for sintering from MgO, leading to a drastic reduction in the CO2 carrying activity (spent sorbent). This paper presents a novel method for the reactivation of spent dolomite sorbents. Notable activity recovery is achieved by ball milling of the spent sorbent with H2O and dry ice. Powder X-ray diffraction (XRD) results confirm the transformation from oxide (CaO/MgO) to carbonate (CaCO3/CaMg(CO3)2), so that the segregated Ca and Mg in spent sorbent are re-mixed at the atomic level, which is mainly responsible for this effective reactivation. Water plays an irreplaceable role in this process by providing a liquid environment to accelerate the diffusion of the reactants and ionic reactions. In addition, thermogravimetric analysis was carried out on a series of samples with different ball-milling times to determine the suitable reactivation conditions for CO2 capture.