Athens has a serious air pollution problem which became evident in the early 1970s. Studies for the years 1975-1982 have indicated a positive association of sulphur dioxide (SO2) with total daily mortality. Since 1983 the pollution profile in Athens has gradually changed but the levels of smoke, SO2 and carbon monoxide (CO) remain relatively high. The association of air pollution with daily all-cause mortality in Athens for the years 1984-1988 was investigated using daily values of SO2, smoke and CO. Autoregressive models with log-transformed daily mortality as the dependent variable, were used to adjust for temperature and relative humidity (both lagged by 1 day), year, season and day of week, as well as for serial correlations in mortality. Graphic analysis revealed non-linear monotonically increasing relationships between total mortality and SO2, smoke and CO, with steeper exposure-response slopes at lower air pollution levels. Air pollution data lagged by 1 day had the strongest association with daily mortality. In three separate autoregression models for log(SO2), log(smoke) and log(CO) the regression coefficients for each were highly statistically significant (P < 0.001). Further multiple regression modelling showed that SO2 and smoke are both independent predictors of daily mortality, though to a lesser extent than temperature and relative humidity. The inclusion of CO in the model did not further improve the prediction of daily mortality. The magnitude of association is small, for instance, a 10% reduction in smoke is estimated to decrease daily mortality by 0.75% (95% confidence interval [CI]: 0.51-0.99). However, it cannot be accounted for by climatic and seasonal effects, so that a causal influence of air pollution on daily mortality seems plausible. These findings suggest that current air pollution levels in Athens (and many other industrialized cities) may be responsible for substantial numbers of premature deaths, and hence remain an important public health issue.