AbstractLime mud, a kind of industrial waste that produced in paper mill, was proposed as CO2 sorbent in calcium looping process. The carbonation performance of the lime mud was investigated in a dual‐fixed bed reactor (DFR) and a thermogravimetric analyzer (TGA). The carbonation kinetics of the lime mud in the chemical reaction controlled stage was analyzed by a surface reaction‐controlled kinetic model. The results show that the lime mud presents much poorer carbonation performance during the chemical reaction controlled stage compared with the limestone, mainly due to the high content of chlorine in the lime mud. A prewash treatment process was used to decrease the chlorine content to mitigate the sintering of the lime mud when calcined at high temperature. After prewash treatment, the prewashed lime mud shows much higher CO2 capture capacity during the chemical reaction controlled stage compared with the lime mud. A prolonged carbonation process successfully further enhances the microstructure and improves the carbonation performance of the prewashed lime mud in the chemical reaction controlled stage. The lime mud can be effectively used as CO2 sorbent in calcium looping process after prewash treatment and the following prolonged carbonation treatment.