We analyzed the 1980 U.S. vital statistics and available ambient air pollution data bases for sulfates and fine, inhalable, and total suspended particles. Using multiple regression analyses, we conducted a cross-sectional analysis of the association between various particle measures and total mortality. Results from the various analyses indicated the importance of considering particle size, composition, and source information in modeling of particle pollution health effects. Of the independent mortality predictors considered, particle exposure measures related to the respirable and/or toxic fraction of the aerosols, such as fine particles and sulfates, were most consistently and significantly associated with the reported SMSA-specific total annual mortality rates. On the other hand, particle mass measures that included coarse particles (e.g., total suspended particles and inhalable particles) were often found to be nonsignificant predictors of total mortality. Furthermore, based on the application of fine particle source apportionment, particles from industrial sources (e.g., from iron/steel emissions) and from coal combustion were suggested to be more significant contributors to human mortality than soil-derived particles.