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The problem of large stockpiles of red mud needs to be solved, and the use of red mud to prepare inorganic fibers is a new way of applying red mud on a large scale. The role of CaO/Al₂O₃ in the melting point and melt structure of red mud was investigated by molecular dynamics simulations and thermodynamic calculations. Liquid phase line temperatures for different CaO/Al₂O₃ systems were calculated using the Factsage program. The radial distribution function and the type of oxygen bonding were used to characterize the effect of different CaO/Al₂O₃ on the structure of the red mud melt. The melting point of MgAl₂O₄ is lower than that of CaTiO₃ due to the fact that the type of oxygen bonding in MgAl₂O₄ is predominantly bridging oxygen bonds. When the red mud system has a low SiO₂ content and CaO/Al₂O₃ is between 0.3 and 3.9, the melting point temperature increases significantly, which is not conducive to the fibrillation of the red mud melt.