The GEOstationary Coastal and Air Pollution Events (GEO-CAPE) Airborne Simulator (GCAS) was developed at NASA’s Goddard Space Flight Center (GSFC) and has flown in multiple field campaigns to perform mapping of the regional-scale EPA criteria pollutants nitrogen dioxide, ozone, and formaldehyde. GCAS will also participate invalidation campaigns for NASA’s Tropospheric Emissions: Monitoring POllution (TEMPO) mission and the Korean Geostationary Environment Monitoring Spectrometer (GEMS) mission, both scheduled to launch in the early 2020s. GCAS houses two commercial Offner-type grating spectrometers that measure backscattered solar spectral radiance from the near-ultraviolet to near-infrared at high spatial resolution (typically 250 meters at 8.5 kilometer altitude). These radiances are used to retrieve spatial and temporal distributions of trace gases relevant to the boundary layer and free tropospheric atmospheric chemistry cycles. In this paper, we describe the field calibration techniques employed to characterize the spectral and temporal radiometric stability of the system during its most recent deployment in the 2018 Long Island Sound Trace Ozone Study (LISTOS) field campaign. Overall measurement uncertainty, retrieval impacts, and lessons learned for future deployments will also be described.