Aerosols are a major source of uncertainty in estimates of anthropogenic effects on global radiative forcing and can pose serious health concerns. While many instrumental techniques capable of analyzing aerosol samples are available, individual-particle spectromicroscopic techniques like the ones presented here are the only ones to offer morphological and compositional measurements together. Studying the composition and mixing state of aerosol populations allowed for important aspects to be uncovered, such as: aerosol source, formation mechanism, hygroscopicity, optical properties, level of aging, and inhalation dangers. Ambient aerosols from the Amazon, both biogenic and anthropogenic, were apportioned based on their individual composition. Recently discovered organic aerosols from the central United States were identified and their chemical properties were characterized. The lead fraction of mixed lead- and zinc-rich particles from Mexico City was speciated to determine the lead’s solubility and possible bioavailability. It is through the use of these powerful spectromicroscopic techniques that a better understanding of complex mixed aerosols was achieved.