Trends in the composition of the lower atmosphere (0–1500 m altitude) and surface air quality over the Baltimore/Washington area and surrounding states were investigated for the period from 1997 to 2011. We examined emissions, ground-level observations and long-term aircraft measurements to characterize trends in air pollution. The USEPA Continuous Emissions Monitoring System (CEMS) program reported substantial decreases in point sources resulting from national and regional control measures; these decreases are definitely reflected in the ground-level observations. The decreasing trend of CO column contents is ~8.0 Dobson Unit (DU) decade<sup>−1</sup>, corresponding to ~350 ppbv decade<sup>−1</sup> in the lower troposphere. Satellite observations of long-term, near-surface CO show ~40% decrease over western Maryland between 2000 and 2011, the same magnitude as indicated by aircraft measurements over upwind regions of Baltimore/Washington aished. After compensating for inter-annual temperature variations, historical aircraft measurements suggest the daily net production of tropospheric ozone over Baltimore/Washington area decreases from ~20 ppbv in the late 1990s to ~7 ppbv in the early 2010s during the ozone season. A decrease in the long-term ozone column content is observed as ~2.0 DU decade<sup>−1</sup> in the lowest 1500 m, corresponding to ~13 ppbv decade<sup>−1</sup> decrease. Back trajectory cluster analysis demonstrates that emissions of air pollutants from Ohio and Pennsylvania through Maryland influence column contents of downwind ozone in the lower atmosphere. The trends of air pollutants reveal the success of regulations implemented over the last decade and the importance of region wide emission controls over the eastern United States.