Air quality management strategies in the US are developed largely from estimates of emissions, some highly uncertain, rather than actual measurements. Improved knowledge based on measurements of real-world emissions is needed to increase the effectiveness of these strategies. Consequently, the objectives of this research were to (1) quantify relationships among urban emissions sources, land use, and demographics, (2) determine the spatial and temporal variability of emissions, and (3) evaluate the accuracy of official emissions estimates. These objectives guided three field campaigns that employed a unique mobile laboratory equipped to measure pollutant fluxes by eddy covariance. The first campaign, conducted in Norfolk, Virginia, represented the first time fluxes of nitrogen oxides (NO_x) were measured by eddy covariance in an urban environment. Fluxes agreed to within 10% of estimates in the National Emissions Inventory (NEI), but were three times higher than those of an inventory used for air quality modeling and planning. Additionally, measured fluxes were correlated with road density and increased development. The second campaign took place in the Tijuana-San Diego border region. Distinct spatial differences in fluxes of carbon dioxide (CO₂), NO_x, and particles were revealed across four sampling locations with the lowest fluxes occurring in a residential neighborhood and the highest ones at a port of entry characterized by heavy motor vehicle traffic. Additionally, observed emissions of NO_x and carbon monoxide were significantly higher than those in emissions inventories, suggesting the need for further refinement of the inventories. The third campaign focused on emissions at a regional airport in Roanoke, Virginia. NOx and particle number emissions indices (EIs) were calculated for aircraft, in terms of grams of pollutant emitted per kilogram of fuel burned. Observed NO_x EIs were ~20% lower than those in an international databank. NO_x EIs from takeoffs were significantly higher than those from taxiing, but relative differences for particle EIs were mixed. Observed NO_x fluxes at the airport agreed to within 25% of estimates derived from the NEI. The results of this research will provide greater knowledge of urban impacts to air quality and will improve associated management strategies through increased accuracy of official emissions estimates. / Ph. D.