During the summer of 2004, extensive wildfires burned in Alaska and western Canada; the fires were the largest on record for Alaska. Smoke from these fires was observed over the continental United States in satellite images, and a variety of chemical tracers associated with the fires were sampled by aircrafts deployed during the International Consortium for Atmospheric Research on Transport and Transformation field experiment. Several recent studies have quantified the impacts of the long-range transport of pollution associated with these fires on tropospheric CO and O₃ levels over the eastern United States. This study quantifies the episodic impact of this pollution transport event on surface-level fine particulate matter (PM_2.5) concentrations over the eastern United States during mid-July 2004, through the complementary use of remotely sensed, aloft, and surface measurements, in conjunction with a comprehensive regional atmospheric chemistry-transport model. A methodology is developed to assimilate MODIS aerosol optical depths in the model to represent the impacts of the fires. The resultant model predictions of CO and PM_2.5 distributions are compared extensively with corresponding surface and aloft measurements. On the basis of the model calculations, a 0.12Tg enhancement in tropospheric PM_2.5 mass loading over the eastern United States is estimated on 19 July 2004 due to the fires. This amount is significantly larger (approximately a factor of 8) than the total daily anthropogenic fine particulate matter emissions for the continental United States. Analysis of measured and modeled PM_2.5 surface-level concentrations suggests that the transport of particulate matter pollution associated with the fires resulted in a 24–42 % enhancement in median surface-level PM_2.5 concentrations across the eastern United States during 19–23 July 2004.