Concentrated animal feeding operations (CAFOs) emit a large number of volatile organic compounds (VOCs) to the atmosphere. In this study, we conducted mobile laboratory measurements of VOCs, methane (CH 4 ) and ammonia (NH 3 ) downwind of dairy cattle, beef cattle, sheep and chicken CAFO facilities in northeastern Colorado using a hydronium ion time-of-flight chemical-ionization mass spectrometer (H 3 O + ToF-CIMS) that can detect numerous VOCs. Regional measurements of CAFO emissions in northeastern Colorado were also performed using the NOAA WP-3D aircraft during the Shale Oil and Natural Gas Nexus (SONGNEX) campaign. Alcohols and carboxylic acids dominate VOC concentrations and the reactivity of the VOCs with hydroxyl (OH) radicals. Sulfur-containing and phenolic species provide the largest contributions to in the odor activity values and the nitrate radical (NO 3 ) reactivity of VOC emissions, respectively. VOC compositions determined from mobile laboratory and aircraft measurements generally agree well with each other. The high time-resolution mobile measurements allow the separation of the sources of VOCs from different parts of the operations occurring within the facilities. We show that the emissions of ethanol concentrations are primarily associated with feed storage and handling. Based on mobile laboratory measurements, we apply a multivariate regression analysis using NH 3 and ethanol as tracers to determine the relative importance of animal-related emissions (animal exhalation and waste) and feed-related emissions (feed storage and handling) for different VOC species. Feed storage and handling contribute significantly to emissions of alcohols, carbonyls, carboxylic acids and sulfur-containing species. Emissions of phenolic species and nitrogen-containing species are predominantly associated with animals and their waste.