Red mud produced in the Bayer process is a hazardous solid waste because of its high alkalinity; however, it is rich in valuable components such as titanium, iron, and aluminum. In this study, a novel calcification–carbonation method was developed to recover alkali and alumina from Bayer red mud under mild reaction conditions. Batch experiments were performed to evaluate the potential effects of important parameters such as temperature, amount of CaO added, and CO_2 partial pressure on the recovery of alkali and alumina. The results showed that 95.2% alkali and 75.0% alumina were recovered from red mud with decreases in the mass ratios of Na_2 O to Fe_2O_3 and of Al_2O_3 to Fe_2O_3 from 0.42 and 0.89 to 0.02 and 0.22, respectively. The processed red mud with less than 0.5wt% Na_2 O can potentially be used as a construction material. Red mud produced in the Bayer process is a hazardous solid waste because of its high alkalinity; however, it is rich in valuable components such as titanium, iron, and aluminum. In this study, a novel calcification-carbonation method was developed to recover alkali and alumina from Bayer red mud under mild reaction conditions. Batch results were obtained from evaluate the potential effects of important parameters such as temperature, amount of CaO added, and CO_2 partial pressure on the recovery of alkali and alumina. alkali and 75.0% alumina were recovered from red mud with decreasing in the mass ratios of Na_2O to Fe_2O_3 and of Al_2O_3 to Fe_2O_3 from 0.42 and 0.89 to 0.02 and 0.22, respectively. The processed red mud with less than 0.5wt% Na_2O can potentially be used as a construction material.