The intake fraction is defined for a specific species and emission source as the ratio of attributable population intake to total emissions. Focusing on California's South Coast Air Basin (SoCAB) as a case study, we combine ambient monitoring data with time-activity patterns to estimate the population intake of carbon monoxide and benzene emitted from motor vehicles during 1996–1999. In addition to exposures to ambient concentrations, three microenvironments are considered in which the exposure concentration of motor vehicle emissions is higher than in ambient air: in and near vehicles, inside a building that is near a freeway, and inside a residence with an attached garage. Incorporating data on motor vehicle emissions estimated by the EMFAC2000 model, we estimate that the 15 million people in the SoCAB inhale 0.003–0.009% (34–85 per million, with a best estimate of 47 per million) of primary, nonreactive compounds emitted into the basin by motor vehicles. This population intake of primary motor vehicle emissions is approximately 50% higher than the average ambient concentration times the average breathing rate, owing to higher concentrations int he three microenvironments and also to the temporal and spatial correlation among breathing rates, concentrations, and population densities. The approach demonstrated here can inform policy decisions requiring a metric of population exposure to airborne pollutants.