Ambient concentrations of 22 volatile organic compounds (VOCs) measured at London Marylebone Road (LMR), an urban traffic site, and London Eltham (LE), an urban background site, were analyzed over a period of 23 years to assess the impact of pollution control strategies. A significant decrease in ambient concentration is seen for the majority of VOCs analyzed with total VOC burden decreasing by 76% and 59% for LMR and LE, respectively, across the period studied. This is likely as a result of legislative controls. This analysis was extended to consider the dominant contribution of VOCs to ozone formation at the sites utilizing photochemical ozone creation potential (POCP) values.Similarly, the overall reactivity of the VOC burden at the sites has resulted in a significant decrease of 11% and 7% per year in ozone formation potential (OFP) for LMR and LE, respectively. At LMR, the declines in OFP for VOCs associated with road traffic emissions are all in good agreement at 11%-13% decrease per year. Reasonable agreement is also seen at LE with a decrease of 6%-11% per year in OFP of the VOCs related to traffic sources. VOCs related to non-traffic sources, namely ethane and propane from natural gas leakage, did not see a significant decline over the study period at either site. The variation and composition of the overall VOC burden was compared across three decadal time periods (1997-2000, 2001-2010, 2011-2019) and saw an increase in significance of these pollutants at both sites. At LMR, ethane and propane moved from the fifth and eleventh largest contributors to total VOC burden in 1997-2000 to the first and second largest contributors in 2011-2019. At LE, a similar trend is seen with ethane and propane becoming the first and second largest contributors in the most recent time period, up from second and eighth at the beginning of the dataset. The similarity between these sites suggests such pollutants are not sufficiently controlled under current legislation. The increase in significance of ethane and propane was mirrored in their contribution to ozone generation potential at both sites but ethene continues to dominate in contribution to OFP. At LMR, etheneThis is an open access article under the terms of the Creative Commons Attribution License, which permits use, distribution and reproduction in any medium, provided the original work is properly cited.