A gap in emission inventories of urban volatile organic compound (VOC) sources, which contribute to regional ozone and aerosol burdens, has increased as transportation emissions in the United States and Europe have declined rapidly. A detailed mass balance demonstrates that the use of volatile chemical products (VCPs)—including pesticides, coatings, printing inks, adhesives, cleaning agents, and personal care products—now constitutes half of fossil fuel VOC emissions in industrialized cities.