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Science for Society Buildings account for a significant fraction of the land area in cities and actively exchange air with their proximate outdoor environments via mechanical ventilation systems. However, the direct impact of buildings on urban air pollution remains poorly characterized. Due to reductions in traffic-associated emissions of volatile organic compounds (VOCs), volatile chemical products, which are widely used inside buildings, have become a major VOC source in urban areas. Indoor-generated VOCs are likely to be an important contributor to the VOC burden of the urban atmosphere, and ventilation systems provide a pathway for VOCs to be released outdoors. Here, we show how modern buildings act as significant emission sources of VOCs for the outdoor environment. Our results demonstrate that future air quality monitoring efforts in cities need to account for direct VOC discharge from buildings in order to capture emerging sources of environmental pollution that can impact the climate and human health. Summary Urban air undergoes transformations as it is actively circulated throughout buildings via ventilation systems. However, the influence of air exchange between outdoor and indoor atmospheres on urban air pollution is not well understood. Here, we quantify how buildings behave as a dynamic source and sink for urban air pollutants via high-resolution online mass spectrometry measurements. During our field campaign in a high-performance office building, we observed that the building continually released volatile organic compounds (VOCs) into the urban air and removed outdoor ozone and fine particulate matter. VOC emissions from people, their activities, and surface reservoirs result in significant VOC discharge from the building to the outdoors. Per unit area, building emissions of VOCs are comparable to traffic, industrial, and biogenic emissions. The building source-sink behavior changed dynamically with occupancy and ventilation conditions. Our results demonstrate that buildings can directly influence urban air quality due to substantial outdoor-indoor air exchange.