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Currently, air pollution is primarily characterized by PM 2.5 and O 3. Therefore, the co-control of PM 2.5 and O 3 has become an important task of atmosphere pollution prevention and control in China. However, few studies have been conducted on the emissions from vapor recovery and processes, which is an important source of VOCs. This paper analyzed the VOC emissions of three vapor process technologies in service stations and first proposed key pollutants for priority control based on the coordinated reactivity of O 3 and SOA. The concentration of VOCs emitted from the vapor processor was 3.14–9.95 g m−3, compared to 631.2–717.8 g m−3 for uncontrolled vapor. Alkanes, alkenes, and halocarbons accounted for a high proportion of the vapor both before and after control. Among the emissions, i -pentane, n -butane, and i -butane were the most abundant species. Then, the species of OFP and SOAP were calculated through the maximum incremental reactivity (MIR) and fractional aerosol coefficient (FAC). The average source reactivity (SR) value of the VOC emissions from three service stations was 1.9 g g−1, while the OFP ranged from 8.2 to 13.9 g m−3 and SOAP ranged from 0.18 to 0.36 g m−3. By considering the coordinated chemical reactivity of O 3 and SOA, a comprehensive control index (CCI) was proposed for the control of key pollutant species that have multiplier effects on environment. For adsorption, trans -2-butene and p -xylene were the key co-control pollutants, while toluene and trans -2-butene were the most important for membrane and condensation + membrane control. A 50% emission reduction of the top two key species that emission account for 4.3% averagely will reduce O 3 by 18.4% and SOA by 17.9%. [Display omitted] • The organized emissions of VOCs from three vapor processors were studied in service stations. • The species composition of VOCs before and after control were analyzed. • The OFP and SOAP were calculated to evaluate the secondary pollution. • The co-control of key pollutants based on SOA and O 3 has great environmental benefits. [ABSTRACT FROM AUTHOR]