We used conventional and environmental transmission electron microscopes to determine morphology, composition, and water uptake of individual natural inorganic aerosol particles collected from industrial pollution plumes and from clean and polluted marine environments. Five particle types are described in detail. They range from relatively insoluble mineral grains to internally mixed particles containing NaCl with other soluble or relatively insoluble material. We studied the hygroscopic behavior of these particles from 0 to 100% relative humidity (RH). Relatively insoluble materials do not take up water over the experimental RH range. Single crystals of NaCl from both natural and laboratory sources have a well-defined deliquescence point of approximately 76% RH at 291 K. NaCl-bearing aggregate particles appear to deliquesce between 74 and 76% RH (same RH within error) when NaCl is internally mixed with relatively insoluble phases, but the particles deliquesce at lower RH when aggregated with other soluble phases such as NaNO3. For all NaCl-bearing particles studied, hygroscopic growth is pronounced above 76% RH, and water uptake by the particles is dominated by the soluble phase. Furthermore, the soluble phase initiating deliquescence controls the locus of further hygroscopic growth of the aggregate particle. Our results demonstrate that composition and mixing state affect water uptake of natural aerosol particles. Furthermore, internally mixed particles are confirmed to deliquesce at lower RH values than predicted from the individual components.