The Atlanta Commuters Exposure (ACE) Study was designed to measure in-cabin exposure to roadway particulate pollution and acute health response in a panel of adults with and without asthma following a 2-h scripted route along major highways in Atlanta. This article focuses on methods and results of both continuous and integrated approaches used to measure the concentration of PM 2.5 mass, particle number concentration (PNC), black carbon (BC) mass, and particle-bound PAHs, in-cabin noise, PM elemental composition, elemental carbon, organic carbon, water-soluble organic carbon (WSOC) content, and speciation of a broad range of organic compounds including alkanes, hopanes, and PAHs. Speciated PM data indicates that in-cabin particles derive from three non-co-varying processes: the resuspension of road dust containing crustal elements and previously-deposited brake pad residue with a contribution of normal fuel combustion, incomplete combustion processes producing PAHs and carbon particles, and particles ablated from brake pads that have not previously deposited to the roadside environment. Most in-cabin pollutants were elevated during the warm season with the notable exception of PNC. PNC was not found to be correlated with most other pollutants. In-cabin concentrations were marginally higher when windows were open.