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In this study, which was a part of the Atmospheric Exchange Over Lakes and Oceans Study (AEOLOS) investigation, the dry deposition fluxes and atmospheric size distributions (ASDs) of mass and crustal metals (aluminum and magnesium) were measured over the southern basin of Lake Michigan (in Chicago, over Lake Michigan, and in South Haven, Michigan). Airborne crustal metals arise primarily from fugitive dust emissions and are associated with the coarse fraction of atmospheric aerosol. Consequently, they can serve as fingerprints for the atmospheric behavior of fugitive dust. The flux of these metals were substantially higher in Chicago than in either South Haven or over Lake Michigan. The measured average mass, aluminum, and magnesium fluxes were 138, 2.23, and 5.32 mg/m2-day in Chicago, 47.8, 0.24, and 0.28 mg/m2-day over Lake Michigan, and 37.4, 0.17, and 0.12 mg/m2-day in South Haven, respectively. The ASDs of crustal metals measured in Chicago had higher concentrations of coarse particles than ASDs measured over Lake Michigan and in South Haven. The calculated flux of metals using a multistep model and dry deposition velocities obtained from the Sehmel-Hodgson model were in general agreement with measured fluxes of crustal metals. Particles >10 μm were found to be responsible for the majority of the flux.