Large scale utilization of high alkalinity red mud generated in Bayer process is becoming a worldwide problem. Aiming at this problem, a novel calcification-carbonation process is proposed. Firstly, red mud was treated with lime, where the silicon phase is converted into hydrogarnet and alkali is removed. Then, calcification residue is decomposed by CO2 and alumina is recovered. The effect of calcification temperature, Ca-Si molar ratio, and liquid-solid ratio on alkali content in calcification process were investigated. The results indicate that the w(Na2O)in red mud reduces from 6.70% to 0.35% at reaction temperature of 160℃, Ca-Si molar ratio of 2.5∶1, liquid-solid ratio of 3∶1. Moreover, the XRD results show that diffraction peak of the alkali in red mud disappears after the calcification transformation, and hydrogarnet is the main phase.