We present the first direct, multisite observations in support of the hypothesis that atmospheric aerosols affect the regional terrestrial carbon cycle. The daytime growing season (summer) CO2 flux observations from six sites (forest, grasslands, and croplands) with collocated aerosol and surface radiation measurements were analyzed for high and low diffuse radiation; effect of cloud cover; and effect of high and low aerosol optical depths (AOD). Results indicate that, aerosols exert a significant impact on net CO2 exchange, and their effect may be even more significant than that due to clouds. The response appears to be a general feature irrespective of the landscape and photosynthetic pathway. The CO2 sink increased with aerosol loading for forest and crop lands, and decreased for grassland. The cause for the difference in response between vegetation types is hypothesized to be canopy architecture.