Airborne observations made on 8 July 2002 over five locations in Virginia and Maryland revealed the presence of two discrete layers of air pollution, one of a smoke plume between ∼2 and 3 km above mean sea level advected from Quebec forest fires and another, underlying plume from fossil fuel combustion. Within the smoke layer, large increases were observed in submicrometer particle numbers, scattering, and absorption as well as ozone (O3) and CO (but not SO2) mixing ratios. The single-scattering albedos (ω0) in the layer between ∼2 and 3 km (mean value at 550 nm = 0.93 ± 0.02) were consistently smaller than those below (mean value at 550 nm = 0.95 ± 0.01). Aerosol optical depth in the lower 3 km of the atmosphere was determined at each of the five locations, and the value at 550 nm varied between 0.42 ± 0.06 and 1.53 ± 0.21. Calculations of clear-sky aerosol direct radiative forcing by the smoke plume using an atmospheric radiative transfer code indicated that the forcing at the top of the atmosphere was small relative to the forcing at the surface. Thus atmospheric absorption of solar radiation was nearly equal to the attenuation at the surface. The net effect was to cool the surface and heat the air aloft. A morning subsidence inversion positioned the smoke in a dense enough layer above the planetary boundary layer that solar heating of the layer maintained the temperature inversion through the afternoon. This created a positive feedback loop that prevented vertical mixing and dilution of the smoke plume, thereby increasing the regional radiative impact.