We report empirical estimates of the fractional solubility of aerosol iron over the Sargasso Sea during periods characterized by high concentrations of Saharan dust (summer 2003) and by low concentrations of aerosols in North American/maritime North Atlantic air masses (spring 2004 and early summer 2004). We observed a strong inverse relationship between the operational solubility of aerosol iron (defined using a flow-through deionized-water leaching protocol) and the total concentration of aerosol iron, whereby the operational solubility of aerosol iron was elevated when total aerosol iron loadings were low. This relationship is consistent with source-dependent differences in the solubility characteristics of our aerosol samples and can be described by a simple mixing model, wherein bulk aerosols represent a conservative mixture of two air mass end-members that carry different aerosol types: “Saharan air,” which contains a relatively high loading of aerosol iron (27.8 nmol Fe m−3) that has a low fractional solubility (0.44%), and “North American air,” which contains a relatively low concentration of aerosol iron (0.5 nmol Fe m−3) that has a high fractional solubility (19%). Historical data for aerosols collected on Bermuda indicate that the low iron loadings associated with North American air masses are typically accompanied by elevated V/Al, Fe/Al, and V/Mn mass ratios in the bulk aerosol, relative to Saharan dust, which are indicative of anthropogenic fuel-combustion products. The identification of similar compositional trends in our Sargasso Sea aerosol samples leads us to suggest that the elevated solubility of iron in the aerosols associated with North American air masses reflects the presence of anthropogenic combustion products, which contain iron that is readily soluble relative to iron in Saharan soil dust. We thus propose that the source-dependent composition of aerosol particles (specifically, the relative proportion of anthropogenic combustion products) is a primary determinant for the fractional solubility of aerosol iron over the Sargasso Sea. This hypothesis implies that anthropogenic combustion emissions could play a significant role in determining the atmospheric input of soluble iron to the surface ocean.