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Methods to radiometrically calibrate a non-imaging airborne visible-to-shortwave infrared (VSWIR) spectrometer to measure the Greenland ice sheet surface are presented. Airborne VSWIR measurement performance for bright Greenland ice and dark bare rock/soil targets is compared against the MODerate resolution atmospheric TRANsmission (MODTRAN®) radiative transfer code (version 6.0), and a coincident Landsat 8 Operational Land Imager (OLI) acquisition on 29 July 2015 during an in-flight radiometric calibration experiment. Airborne remote sensing flights were carried out in northwestern Greenland in preparation for the Ice, Cloud, and land Elevation Satellite 2 (ICESat-2) laser altimeter mission. A total of nine science flights were conducted over the Greenland ice sheet, sea ice, and open-ocean water. The campaign's primary purpose was to correlate green laser pulse penetration into snow and ice with spectroscopic-derived surface properties. An experimental airborne instrument configuration that included a nadir-viewing (looking downward at the surface) non-imaging Analytical Spectral Devices (ASD) Inc. spectrometer that measured upwelling VSWIR (0.35 to 2.5 µm) spectral radiance (Wm-2sr-1µm-1) in the two-color Slope Imaging Multi-polarization Photon-Counting Lidar's (SIMPL) ground instantaneous field of view, and a zenith-viewing (looking upward at the sky) ASD spectrometer that measured VSWIR spectral irradiance (W m−2 nm−1) was flown. National Institute of Standards and Technology (NIST) traceable radiometric calibration procedures for laboratory, in-flight, and field environments are described in detail to achieve a targeted VSWIR measurement requirement of within 5 % to support calibration/validation efforts and remote sensing algorithm development. Our MODTRAN predictions for the 29 July flight line over dark and bright targets indicate that the airborne nadir-viewing spectrometer spectral radiance measurement uncertainty was between 0.6 % and 4.7 % for VSWIR wavelengths (0.4 to 2.0 µm) with atmospheric transmittance greater than 80 %. MODTRAN predictions for Landsat 8 OLI relative spectral response functions suggest that OLI is measuring 6 % to 16 % more top-of-atmosphere (TOA) spectral radiance from the Greenland ice sheet surface than was predicted using apparent reflectance spectra from the nadir-viewing spectrometer. While more investigation is required to convert airborne VSWIR spectral radiance into atmospherically corrected airborne surface reflectance, it is expected that airborne science flight data products will contribute to spectroscopic determination of Greenland ice sheet surface optical properties to improve understanding of their potential influence on ICESat-2 measurements.