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The fire influence on regional to global environments and air quality (FIREX-AQ) field campaign was conducted during August 2019 to investigate the impact of wildfire and biomass smoke on air quality and weather in the continental United States. One of the campaign&#x0027;s scientific objectives was to estimate the composition of emissions from wildfires. Ultraspectrally resolved infrared radiance measurements from aircraft and&#x002F;or satellite observations contain information on tropospheric carbon monoxide (CO) as well as other trace species present in fire emissions. A methodology for retrieving tropospheric CO from such remotely sensed spectral data has been developed for the National Airborne Sounder Testbed-Interferometer (NAST-I) and is applied herein. Retrievals based on NAST-I measurements are used to demonstrate CO retrieval capability and characterize fire emissions. NAST-I remotely sensed CO from ER-2 flights are evaluated with concurrent <italic>in situ</italic> measurements from the differential absorption carbon monoxide measurements flown on the NASA DC-8 aircraft. Enhanced CO emissions along with plume evolution and transport from the fire ground site locations were captured by moderate vertical and high horizontal resolution observations obtained from the NAST-I IR spectrometer; these were intercompared and verified by the cloud physics lidar and the enhanced MODIS airborne simulator also hosted on the NASA ER-2 aircraft. This study will be beneficial to the science community for studying wildfire-related topics and understanding similar remotely sensed observations from satellites, along with helping to address the broader FIREX-AQ experiment objectives of investigating the impact of fires on air quality and climate.