A method for recovering alkali and aluminum during treatment of Bayer red mud using a calcification-carbonation method, including steps of mixing the Bayer red mud with calcium aluminate or with calcium aluminate and lime, performing calcification dealkalization conversion in a high-concentration alkaline liquor, and carbonizing the calcified residues produced during dealkalization to obtain carbonized residues; and then performing low-temperature aluminum dissolution, aluminum precipitation and the like to obtain calcium aluminate products, which is returned to the calcification dealkalization conversion of the red mud for recycling. Part of an alkali-containing and aluminum-containing liquid phase after calcification dealkalization conversion can be used as supplementary alkali in the Bayer production course for recycling. The method is energy-saving and environmentally-friendly, and allows recovering alkali and aluminum from the red mud and harmless treatment of the Bayer red mud.