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Fine particulate matter (PM2.5) and volatile organic compounds (VOCs) are associated with adverse health effects and show spatial variation in three dimensions. The present study attempted to evaluate source contributions of PM2.5 and toxic VOCs in a metropolitan area focusing on the associated vertical variations. A special emphasis is put on the effects of the elevated expressway on the vertical variability of contribution estimates of the identified sources. Nine source factors, i.e., soil dust, sea salt/oil combustion, secondary nitrate, industrial emission, aged VOCs/secondary aerosol, traffic-related I, solvent use/industrial process, secondary sulfate, and traffic-related II, were identified using positive matrix factorization (PMF). The main contributors to PM2.5 were secondary sulfate (19.1%) and traffic-related emissions (traffic-related I and II, 16.1%), whereas the largest contributors to VOCs were traffic-related emissions (37.6%). The influence of the elevated expressway is suggested to be particularly critical on vertical variations of traffic-related emissions, including aging and secondary formation of locally accumulated air pollutants near roads. Increasing the building porosity under the viaduct could reduce the accumulation of air pollutants caused by the shelter effect. Additionally, in-street barriers would be beneficial in reducing population exposure to traffic-related emissions by altering the airflows near roads. [ABSTRACT FROM AUTHOR]