Although it is known that soot particles are emitted in large quantities to the atmosphere, our understanding of their environmental effects is limited by our knowledge of how their composition is subsequently altered through atmospheric processing. Here we present an on-line mass spectrometric study of the changing chemical composition of hydrocarbon soot particles as they are oxidized by gas-phase ozone, and we show that the surface-mediated loss rates of adsorbed polycyclic aromatic hydrocarbons in soot are directly connected to a significant increase in the particle redox cycling abilities. With redox cycling implicated as an oxidative stress mechanism that arises after inhalation of atmospheric particles, this work draws a quantitative connection between the detailed heterogeneous chemistry occurring on atmospheric particles and a potential toxic mechanism attributable to that aerosol.