Authoritative, trustworthy, continual, automatic hourly air quality monitoring is a relatively recent innovation. The task of reliably identifying long-term trends in air quality is therefore very challenging, as well as complex. Ports are major sources of atmospheric pollution, which is linked to marine traffic and increased road traffic congestion. This study investigated the long-term trends and drivers of atmospheric pollution in the port cities of Houston, London, and Southampton in 2000–2019. Authoritative air quality and meteorological data for seven sites at these three locations were meticulously selected alongside available traffic count data. Data were acquired for sites close to the port and sites that were near the city centre to determine whether the port emissions were influencing different parts of the city. Openair software was used for plots and statistical analyses. Pollutant concentrations at Houston, Southampton and Thurrock (London) slowly reduced over time and did not exceed national limits, in contrast to NO2 and PM10 concentrations at London Marylebone Road. Drivers of atmospheric pollution include meteorology, geographical and temporal variation, and traffic flow. Statistically significant relationships (p < 0.001) between atmospheric pollution concentration and meteorology across most sites were found, but this was not seen with traffic flows in London and Southampton. However, port emissions and the other drivers of atmospheric pollution act together to govern the air quality in the city.