Atmospheric aerosols scatter and potentially absorb incoming solar radiation, thereby reducing the total amount of radiation reaching the surface and increasing the fraction that is diffuse. The partitioning of incoming energy at the surface into sensible heat flux and latent heat flux is postulated to change with increasing aerosol concentrations, as an increase in diffuse light can reach greater portions of vegetated canopies. This can increase photosynthesis and transpiration rates in the lower canopy and potentially decrease the ratio of sensible to latent heat for the entire canopy. Here, half-hourly and hourly surface fluxes from six Flux Network (FLUXNET) sites in the coterminous United States are evaluated over the past decade (2000–08) in conjunction with satellite-derived aerosol optical depth (AOD) to determine if atmospheric aerosols systematically influence sensible and latent heat fluxes. Satellite-derived AOD is used to classify days as high or low AOD and establish the relationship between aerosol concentrations and the surface energy fluxes. High AOD reduces midday net radiation by 6%–65% coupled with a 9%–30% decrease in sensible and latent heat fluxes, although not all sites exhibit statistically significant changes. The partitioning between sensible and latent heat varies between ecosystems, with two sites showing a greater decrease in latent heat than sensible heat (Duke Forest and Walker Branch), two sites showing equivalent reductions (Harvard Forest and Bondville), and one site showing a greater decrease in sensible heat than latent heat (Morgan–Monroe). These results suggest that aerosols trigger an ecosystem-dependent response to surface flux partitioning, yet the environmental drivers for this response require further exploration.