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Ground-level ozone (O3), which is mainly from the photochemical reactions of NOx and volatile organic compounds (VOCs), has become a crucial pollutant obstructing air quality improvement in China. Understanding the composition, temporal variability and source apportionment of VOCs is necessary for determining effective control measures to minimize VOCs and their related photochemical pollution. To provide a comprehensive analysis of VOC sources and their contributions to ozone formation in the city of Chengdu—a megacity with the highest rates of industrial and economic development in southwest China—we conducted a one-month monitoring project at three urban sites (Shuangliu, Xindu, Junpingjie; SL, XD and JPJ, respectively) along the main north–south meteorological transport channel before and during the implemented control measures. Alkanes were the dominant group at each site, contributing to around 50% of the observed total VOCs, followed by oxygen-containing VOCs (OVOCs), aromatics, halohydrocarbons and alkenes. During the control period, the mixing ratios of most measured VOC species decreased, and O3 concentrations were down by at least 20%. VOC species experiencing the most effect from control were aromatics and OVOCs, which had higher O3 formation reactivity. This indicated that the control policies had significant influence on reductions of reactive VOC species. We also identified VOC sources at SL and XD using positive matrix factorization (PMF) and assessed their contributions to photochemical O3 formation by calculating the O3 formation potential (OFP) based on mass concentrations and maximum incremental reactivity of related VOCs. Five dominant VOC sources were identified, with the highest contributions from vehicular exhaust and fuel evaporation before control, followed by solvent utilization, biogenic background and secondary formation, and industrial emissions. Contribution from vehicular exhaust was reduced the most at SL, while at XD, secondary formation VOCs decreased significantly. VOCs from vehicular and industrial emissions and solvent utilization were found to be the dominant precursors for OFPs, particularly the species of xylenes, toluene and propene. Our results therefore suggest that priority should be given to the alleviation of photochemical pollutants for effective control of O3 formation in Chengdu. The findings from this work have important implications for formulating effective emission control policies in Chengdu. [ABSTRACT FROM AUTHOR]