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Bauxite residue (red mud) generated during alumina production is a highly alkaline solid waste. The red mud is mainly stored on land, but it can cause harm to the surrounding environment and human health. The transformation of red mud into soil is a feasible method for the large-scale disposal of red mud, but alkali removal is the key process that controls the transformation of red mud into soil. In this study, the calcification dealkalization of red mud with a small particle size was carried out below 100 °C. The results show that the sodium in red mud is predominately distributed in small particles, mainly because the lattice alkali and alkali present between the crystals are exposed to the surface of red mud particles by ball milling. The dealkalization process was controlled by the internal diffusion of the shrinking-core model (SCM), and the apparent activation energy was 23.55 kJ/mol. The dealkalization rate and the Na₂O content of dealkalized red mud reached 92.44% and 0.61%, respectively. The dealkalization rate increased with increasing reaction time, reactant concentration, and leaching temperature, and this result was consistent with the results of the kinetic study. In addition, calcification enhances the flocculation of particles, so the filtration performance of red mud improved.