Single particle analysis of individual sea spray aerosol particles shows that cations (Na+, K+, Mg2+, and Ca2+) within individual particles undergo a spatial redistribution after heterogeneous reaction with nitric acid, along with the development of a more concentrated layer of organic matter at the surface of the particle. These data suggest that specific ion and aerosol pH effects play an important role in aerosol particle structure in ways that have not been previously recognized.