Ground surface ozone (O3) is an emerging concern in China due to its complex formation process. In August 2020, field measurements of O3, NOx, and volatile organic compounds (VOCs) were carried out in Hefei’s western suburbs. The pollution features of VOCs and O3 formation were thoroughly analyzed. The total VOC concentration was 42.26 ppb, with the dominant contributor being oxygenated VOCs (OVOCs). Seven emission sources were recognized using the positive matrix factorization (PMF) model, including aged air masses, combustion sources, fuel evaporation, industrial emissions, vehicular emission, solvent utilization, and biogenic emission. Ozone generation mainly occurred under an NOx-limited regime based on the zero-dimensional box model analysis. According to the scenario analysis, the 13% cut in O3 might be achieved by the 10% and 30% reduction in NOx and VOCs, respectively. The O3 budget analysis demonstrates its high ozone production rate during the pollution period. The influence of regional transport cannot be ignored for high O3 pollution. This paper provides scientific evidence for O3 production and the strategies of reducing O3 by controlling its precursors.