The atmospheric aging of soot can significantly modify its composition and microstructure, likely leading to changes in its effects on climate and health. The photochemical aging process of soot by O 3 under simulated sunlight was investigated using in situ attenuated total internal reflection infrared spectroscopy.Simulated sunlight could markedly enhance the aging of soot by O 3 , which produced various oxygen containing species such as lactones, anhydrides, ketones and aldehydes. Elemental carbon (EC) showed minor reactivity toward O 3 . The organic carbon (OC), which was mainly composed of various polycyclic aromatic hydrocarbons (PAHs) and some unidentified components, played a key role in the photochemical aging of soot by O 3 . The kinetics of aromatic species on soot can be well described by a pseudo-first order reaction. The fitting results of the pseudo first-order rate constant (k 1,obs ) as a function of O 3 concentration demonstrated that the photochemical reaction of soot with O 3 followed the Langmuir-Hinshelwood mechanism.