Atmospheric deposition of aerosol iron (Fe) can stimulate marine primary productivity by supplying dissolved Fe (d-Fe) to the surface ocean, thereby potentially influencing the global climate. Aerosol Fe solubility (Fe<sub>sol</sub>%) is closely linked to its bioavailability, and previous studies have shown that Fe<sub>sol</sub>% generally increases as aerosol Fe concentration decreases. However, the mechanism underlying this widely observed inverse relationship remains unresolved. In this study, aerosol observations from East Asia, the North and South Pacific, and the Atlantic were compiled, and the ratios of total Fe to total Al (T-Fe/T-Al) and dissolved Fe to dissolved Al ([d-Fe]/[d-Al]) were used to estimate the contributions of mineral-derived and anthropogenic Fe to aerosol d-Fe, as well as the Fe<sub>sol</sub>% of each source fraction. Aerosol d-Fe was found to be derived predominantly from mineral dust in many oceanic regions. In addition, both mineral-derived Fe and anthropogenic Fe showed inverse relationships between concentration and solubility. If the inverse relationship between Fe concentration and Fe<sub>sol</sub>% were controlled mainly by simple two-component mixing between low-solubility mineral particles and highly soluble anthropogenic Fe, the Fe<sub>sol</sub>% of each source fraction would not be expected to vary systematically with concentration. Instead, the results suggest that atmospheric chemical processing, together with depositional removal during transport, progressively increases the solubility of Fe remaining in aerosol particles. The ability to estimate the sources and dissolution processes of aerosol Fe from such fundamental concentration data may help improve the parameterization of aerosol Fe dissolution in global climate models.