The invention relates to the field of aluminum smelting, in particular to a dealkalization method of red mud by the Bayer process, comprising: a, taking red mud; b, taking calcium oxide-containing materials, strong oxidants, and fluorides and putting them into enhanced diffusion of red mud slurry In the container, control the CaO in the calcium oxide-containing material and the Na in the solid phase of the red mud 2 The weight ratio of O is 2 to 6, the addition of strong oxidant is 0 to 0.1% of the content of sodium oxide in red mud, and the addition of fluoride is 0 to 0.1% of the content of sodium oxide in red mud to obtain mixed pulp residue; c, Atmospheric pressure dealkalization reaction, put the mixed pulp slag obtained in step b into a stirred atmospheric pressure dealkalization reactor for dealkalization reaction, the reaction temperature is 50-102°C, the liquid-solid ratio is 3-8, and the reaction time is greater than 3h ; d, separation and washing, the separated alkali-containing solution is returned to the alumina production process, and the separated low-alkali red mud is sent to the storage yard for storage, which can reduce the alkali content in the discharged red mud to less than 1%, and does not produce other hazardous waste.