The aim of the present study is to assess whether certain ecophysiological responses (contents of total phenols, total proanthocyanidins, and total and simple flavonols), in the needles of Aleppo pines (Pinus halepensis Mill.) may be valid bioindicators for the assessment of the air quality. Samples were taken at five natural sites polluted by various pollutants (NO, NO2, other NOx, SO2, and O3). The results show a decrease in total phenol concentrations with levels of nitrogen oxide pollutions (significant negative correlations between the total phenol concentrations and concentrations of NO, NO2, and other NOx). Total flavonoids (total flavonols and proanthocyanidins) are useful bioindicators for ozone pollution (significant negative correlations between total proanthocyanidins and the concentrations of ozone and significant positive correlations between total flavonols and the ozone pollution). Sulfur dioxide pollution is distinguished by low concentrations in quercetin, isorhamnetin, and kaempferol (significant negative correlations between these simple flavonols and the concentrations of SO2). This work confirms the strong interest of using the phenolic compounds of Pinus halepensis as biological indicators of air quality.