Organic aerosol (OA) is a major component of fine particulate matter (PM2.5) in urban environments. We performed in-motion ambient sampling from a mobile platform with an aerosol mass spectrometer (AMS) to investigate the spatial variability and sources of OA concentrations in Pittsburgh, Pennsylvania, a midsize, largely postindustrial American city. To characterize the relative importance of cooking and traffic sources, we sampled in some of the most populated areas (∼18 km2) in and around Pittsburgh during afternoon rush hour and evening mealtime, including congested highways, major local roads, areas with high densities of restaurants, and urban background locations. We found greatly elevated OA concentrations (10s of μg m–3) in the vicinity of numerous individual restaurants and commercial districts containing multiple restaurants. The AMS mass spectral information indicates that majority of the high concentration plumes (71%) were from cooking sources. Areas containing both busy roads and restaurants had systematically higher OA concentrations than areas with only busy roads and urban background locations. Elevated OA concentrations were measured hundreds of meters downwind of some restaurants, indicating that these sources can influence air quality on neighborhood scales. Approximately 20% of the population (∼250 000 people) in the Pittsburgh area lives within 200 m of a restaurant; therefore, restaurant emissions are potentially an important source of outdoor PM exposures for this large population.