We conducted a systematic review of all studies published between 1950 and 2007 of associations between long-term exposure to ambient air pollution and the risks in adults of nonaccidental mortality and the incidence and mortality from cancer and cardiovascular and respiratory diseases. We searched bibliographic databases for cohort and case-control studies, abstracted characteristics of their design and conduct, and synthesized the quantitative findings in tabular and graphic form. We assessed heterogeneity, estimated pooled effects for specific pollutants, and conducted sensitivity analyses according to selected characteristics of the studies. Our analysis showed that long-term exposure to PM2.5 increases the risk of nonaccidental mortality by 6% per a 10 microg/m3 increase, independent of age, gender, and geographic region. Exposure to PM2.5 was also associated with an increased risk of mortality from lung cancer (range: 15% to 21% per a 10 microg/m3 increase) and total cardiovascular mortality (range: 12% to 14% per a 10 microg/m3 increase). In addition, living close to busy traffic appears to be associated with elevated risks of these three outcomes. Suggestive evidence was found that exposure to PM2.5 is positively associated with mortality from coronary heart diseases and exposure to SO2 increases mortality from lung cancer. For the other pollutants and health outcomes, the data were insufficient data to make solid conclusions.