Abstract: Phyllosilicate minerals have special properties and have attracted much attention in research in the fields of mineral flotation and mineral materials applications. Molecular simulation, as an efficient analytical prediction tool, can understand the nature of phyllosilicate minerals from a microscopic perspective. The current status of molecular simulation studies on five typical phyllosilicate minerals, namely talc, serpentine, montmorillonite, kaolinite, and mica, is reviewed, which mainly include interlayer hydration, mineral adsorption of flotation reagents, and other pollutants, with the aim of further understanding of phyllosilicate minerals and better separating and utilizing phyllosilicate minerals.