Tobacco smoke residues lingering in the indoor environment, also termed thirdhand smoke (THS), can be a source of long-term exposure to harmful pollutants. THS composition is affected by chemical transformations and by air-surface partitioning over time scales of minutes to months. This study identified and quantified airborne THS pollutants available for respiratory exposure, identified potential environmental tracers, and estimated health impacts to nonsmokers. In a ventilated 18 m(3) laboratory chamber, six cigarettes were machine-smoked, and levels of particulate matter (PM2.5) and 58 volatile organic compounds (VOCs) were monitored during an aging period of 18 h. Results were compared with field measurements taken in a smoker's home 8 h after the last cigarette had been smoked. Initial chamber levels of individual VOCs in freshly emitted secondhand smoke (SHS) were in the range of 1-300 μg m(-3). The commonly used SHS tracers 3-ethenylpyridine (3-EP) and nicotine were no longer present in the gas phase after 2 h, likely due mostly to sorption to surfaces. By contrast, other VOCs persisted in the gas phase for at least 18 h, particularly furans, carbonyls, and nitriles. The concentration ratio of acetonitrile to 3-EP increased substantially with aging. This ratio may provide a useful metric for differentiating freshly emitted (SHS) from aged smoke (THS). Among the 29 VOCs detected in the smoker's home at moderate to high concentrations, 18 compounds were also detected in simultaneously sampled outdoor air, but acetonitrile, 2-methyl furan, and 2,5-dimethyl furan appeared to be specific to cigarette smoke. The levels of acrolein, methacrolein, and acrylonitrile exceeded concentrations considered harmful by the State of California. An initial exposure and impact assessment was conducted for a subset of pollutants by computing disability-adjusted life years lost, using available toxicological and epidemiological information. Exposure to PM2.5 contributed to more than 90% of the predicted harm. Acrolein, furan, acrylonitrile, and 1,3-butadiene were considered to be the most harmful VOCs. Depending on which criteria are used to establish the separation between SHS and THS, 5-60% of the predicted health damage could be attributed to THS exposure. Benefits and limitations of this approach are discussed.