Due to the adverse effect of atmospheric aerosols on public health and their ability to affect climate, extensive research has been undertaken in recent decades to understand their sources and sinks, as well as to study their physical and chemical properties. Atmospheric aerosols are important players in the Earth’s radiative budget, affecting incoming and outgoing solar radiation through absorption and scattering by direct and indirect means. While the cooling properties of pure inorganic aerosols are relatively well understood, the impact of organic aerosols on the radiative budget is unclear. Additionally, organic aerosols are transformed through chemical reactions during atmospheric transport. The resulting complex mixture of organic aerosol has variable physical and chemical properties that contribute further to the uncertainty of these species modifying the radiative budget. Correlations between oxidative processing and increased absorptivity, hygroscopicity, and cloud condensation nuclei activity have been observed, but the mechanisms behind these phenomena have remained unexplored. Herein, we review environmentally relevant heterogeneous mechanisms occurring on interfaces that contribute to the processing of aerosols. Recent laboratory studies exploring processes at the aerosol–air interface are highlighted as capable of generating the complexity observed in the environment. Furthermore, a variety of laboratory methods developed specifically to study these processes under environmentally relevant conditions are introduced. Remarkably, the heterogeneous mechanisms presented might neither be feasible in the gas phase nor in the bulk particle phase of aerosols at the fast rates enabled on interfaces. In conclusion, these surface mechanisms are important to better understand how organic aerosols are transformed in the atmosphere affecting the environment. View Full-Text