High-resolution measurements of sulfur dioxide (SO2), nitric acid (HNO3), and hydrochloric acid (HCl) were conducted in Athens, Greece, from 2014 to 2016 via a wet rotating annular denuder system paired with an ion chromatograph. Decreased mean annual levels of SO2 and HNO3 (equal to 3.3 ± 4.8 μg m−3 and 0.7 ± 0.6 μg m−3, respectively) were observed relative to the past, whereas for HCl (mean of 0.4 μg m−3 ) no such comparison was possible as the past measurements are very scarce. Regional and local emission sources regulated the SO2 levels and contributed to both the December and the July maxima of 6.6 μg m−3 and 5.5 μg m−3, respectively. Similarly, the significant enhancement at noon and during the winter nighttime was due to transported SO2 and residential heating, respectively. The oxidation of NO2 by OH radicals and the heterogeneous reactions of HNO3 on sea salt seemed to drive the HNO3 and HCl formation, respectively, whereas nighttime biomass burning affected only the former by almost 50%. During summer, the sulfate anions dominated over the SO2, in contrast to the chloride and nitrate ions that prevailed during the winter and were linked to the aerosol acidity that influences their lifetime as well as their impact on ecosystems.