Samples of soil, iron ore, and airborne particulate matter (size <10 μm) were analyzed with the main goal of investigating the differentiating physicochemical properties of their ferruginous compounds. These data were used to identify whether the sources of airborne particulate matter in the metropolitan area of Belo Horizonte, Minas Gerais, Brazil, are either from natural origin, as, for instance, re-suspension of particles from soil, or due to anthropogenic activities, meaning that it would be originated from the many iron ore minings surrounding the metropolitan area. Numerical simulations were used to model the atmospheric dispersion of the airborne particulate matter emitted by iron mining located at the Iron Quadrangle geodomain, Minas Gerais. Results from these numerical simulations supported identifying the sites with the highest concentrations of airborne particulate matter in the metropolitan area. Samples of these suspended materials were collected at the selected sites by using high-volume air samplers. The physicochemical features of the solid materials were assessed by X-ray fluorescence, X-ray diffraction, magnetometry, and Fe Mössbauer spectroscopy. The soil materials were found to be rich in quartz, aluminum, organic matter, and low contents of iron, mainly as low crystalline iron oxides. The samples of the iron ores, on the other hand, contain high concentration of iron, dominantly as relatively pure and crystalline hematite (α-FeO). The samples of the airborne particulate matter are rich in iron, mainly as hematite, but contained also quartz, aluminum, and calcium. Mössbauer spectroscopy was used to evaluate the hyperfine structure of Fe of the hematite both from the iron ore and the soil samples. The structural characteristics of the hematite of these particulate materials were further explored. The direct influence of the iron ore mining on the composition of the airborne particulate matter was clearly evidenced based on the trace ability of hematite to its source of emission. Even the atmospheric air on regions relatively far away from the mining activities is also significantly influenced.