This paper presents laboratory and in-flight radiometric methods to calibrate and deploy a full-spectrum non-imaging airborne visible-to-shortwave infrared (VSWIR) spectrometer to measure polar ice sheet surface optical properties. Using an atmospheric radiative transfer model and coincident Landsat 8 multispectral image, this study concluded that it is possible to measure bright Greenland ice and dark bare rock/soil targets at an airborne remote sensing uncertainty of between 0.6 and 4.7.