Long-term trends in observed carbon monoxide (CO) concentrations were analyzed in seven major South Korean cities from 1989 to 2013. Temporal trends were evident on seasonal and annual timescales, as were spatial gradients between the cities. As CO levels in the most polluted cities decreased significantly until the early 2000s, the data were arbitrarily divided into two time periods (I: 1989–2000 and II: 2001–2013) for analysis. The mean CO concentration of period II was about 50% lower than that of period I. Long-term trends of annual mean CO concentrations, examined using the Mann–Kendall (MK) method, confirm a consistent reduction in CO levels from 1989 to 2000 (period I). The abrupt reduction in CO levels was attributed to a combination of technological improvements and government administrative/regulatory initiatives (e.g., emission mitigation strategies and a gradual shift in the fuel/energy consumption mix away from coal and oil to natural gas and nuclear power).