Atmospheric aerosols are of significant environmental importance, due to their effects on air quality, as well as their ability to alter the planet’s radiative balance. Recent studies characterizing the effects of climate change on air quality and the broader distribution of aerosols in the atmosphere show significant, but inconsistent results, including the sign of the effect. Using a suite of state-of-the-art climate models, we show that climate change is associated with a negative aerosol–climate feedback of −0.02 to −0.09 W m−2 K−1 for direct radiative effects, with much larger values likely for indirect radiative effects. This is related to an increase in most aerosol species, particularly over the tropics and Northern Hemisphere midlatitudes, largely due to a decrease in wet deposition associated with less large-scale precipitation over land. Although simulation of aerosol processes in global climate models possesses uncertainty, we conclude that climate change may increase aerosol burden and surface concentration, which may have implications for future air quality.