The exploitation of iron ore could cause heavy metals pollution in the soils, which threatens the ecosystem and human health. In this study, soil, stream sediment, tailings, rock, and atmospheric deposition samples were collected from an iron mine in Baotou City. The concentrations of As, Cd, Cr, Cu, Hg, Ni, Pb, Zn, Al2O3, CaO, K2O, MgO, Na2O, SiO2, and Fe2O3, as well as the mineral composition and heavy metal speciation of the samples, were analyzed for pollution assessment and source identification of heavy metals. The results reveal that the concentration of Cu in the soils was significantly higher than the background value, and an unpolluted to moderately polluted state was the main pollution level. By analyzing the relationship between Cu/Al2O3 and CaO in different samples, as well as the characteristics of the chemical index of alteration (CIA), mineral composition, and the chemical speciation of Cu in soils and profiles, the results suggest that tailings were the source of Cu pollution in soils. The distribution characteristics of Cu and CaO in stream sediments indicated that hydraulic transport may be one of the main migration pathways. In addition, wind transport may also be a pathway of migration.