A multispectral scanning spectrometer was used to obtain measurements of the bidirectional reflectance and brightness temperature of clouds, sea ice, snow, and tundra surfaces at 50 discrete wavelengths between 0.47 and 14.0 μm. These observations were obtained from the NASA ER-2 aircraft as part of the First ISCCP (International Satellite Cloud Climatology Project) Regional Experiment (FIRE) Arctic Clouds Experiment, conducted over a 1600 km × 500 km region of the north slope of Alaska and surrounding Beaufort and Chukchi Seas between 18 May and 6 June 1998. Multispectral images in eight distinct bands of the Moderate Resolution Imaging Spectroradiometer (MODIS) Airborne Simulator (MAS) were used to derive a confidence in clear sky (or alternatively the probability of cloud) over five different ecosystems. Based on the results of individual tests run as part of this cloud mask, an algorithm was developed to estimate the phase of the clouds (liquid water, ice, or undetermined phase). Finally, the cloud optical thickness and effective radius were derived for both water and ice clouds that were detected during one flight line on 4 June. This analysis shows that the cloud mask developed for operational use on MODIS, and tested using MAS data in Alaska, is quite capable of distinguishing clouds from bright sea ice surfaces during daytime conditions in the high Arctic. Results of individual tests, however, make it difficult to distinguish ice clouds over snow and sea ice surfaces, so additional tests were added to enhance the confidence in the thermodynamic phase of clouds over the Chukchi Sea. The cloud optical thickness and effective radius retrievals used three distinct bands of the MAS, with a recently developed 1.62- and 2.13-μm-band algorithm being used quite successfully over snow and sea ice surfaces. These results are contrasted with a MODIS-based algorithm that relies on spectral reflectance at 0.87 and 2.13 μm.