Bauxite tailings slurry is a type of solid waste produced in the process of bauxite washing and beneficiation. It has poor engineering properties, that is, self-consolidation settlement unusually cannot be completed during several decades. To investigate the sedimentation properties of bauxite tailings, bauxite tailings slurry, phyllite residual soil, and kaolinite, we conduct sedimentation tests on these materials in varying pH and salt solution environments. The influence mechanism of the surface electrical properties of clay particles on the settlement of tailings slurry is investigated using the zeta potential test. The findings reveal that increases in the cation concentration and valence state lead to compression of the electric double layer on the surface of three types of soil particles, resulting in a decline in the repulsive potential energy and an increase in the gravitational potential energy. This in turn contributes to a reduction in the settling stable void ratio. As the pH increases, the zeta potentials of the three soils gradually decrease from positive to negative. A change in the pH at the isoelectric point, PZCedge, triggers the transformation of the kaolinite mineral arrangement. When the pH is either greater than or less than the isoelectric point, an increase or decrease in the pH results in expansion of the electric double layer of the clay particles and an increase in the pore content. The results of this study suggest that bauxite tailings mud is more likely to settle in an acidic environment than in an alkaline environment, thus an acidic settling environment should be utilized for bauxite tailings produced in industrial production.