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The efficient dispersion of particles is a prerequisite for the efficient flotation of fine smithsonite. However, unavoidable ions (Ca2+) in the pulp have become a challenge for the efficient separation of fine smithsonite, due to the high content of pulp and small radius of hydrated ions. Therefore, the dispersion behavior and mechanism of Ca2+ action on smithsonite are important for improving the efficiency of smithsonite flotation. In this study, the effects of Ca2+ on the dispersion behavior of fine smithsonite were studied using a turbidity test. The results showed that the dispersion behavior of smithsonite was good in the absence of Ca2+ at a range of pH = 4–12. However, the measured turbidity values of smithsonite decreased with the addition of calcium ions. In particular, the dispersion behavior of smithsonite became worse at pH > 10. Zeta potential test results showed that the smithsonite's surface potential shifted positively, and the absolute value of potential decreased in the presence of Ca2+. The results of X-ray photoelectron spectroscopy (XPS) and scanning electron microscopy (SEM) analysis showed that calcium ions were adsorbed on the smithsonite surface, which may have caused ion exchange or the generation of calcium hydroxide precipitation leading to particle coalescence behavior. The calculations of solution chemistry and DLVO theory indicated that calcium ions adsorbed on the surface of smithsonite to form Ca(OH)+ or precipitation, which reduced the potential energy of interparticle interactions and led to the disruption of dispersion behavior of smithsonite. [ABSTRACT FROM AUTHOR]