The Moderate Resolution Imaging Spectroradiometer (MODIS) Airborne Simulator (MAS) and MODIS/Advanced Spaceborne Thermal Emission and Reflection Radiometer (ASTER) Airborne Simulator (MASTER) were used to obtain measurements of the bidirectional reflectance and brightness temperature of clouds at 50 discrete wavelengths between 0.47 and 14.2 mm (12.9 mm for MASTER). These observations were obtained from the NASA ER‐2 aircraft as part of the Tropical Composition, Cloud and Climate Coupling (TC4) experiment conducted over Central America and surrounding Pacific and Atlantic Oceans between 17 July and 8 August 2007. Multispectral images in eleven distinct bands were used to derive a confidence in clear sky (or alternatively the probability of cloud) over land and ocean ecosystems. Based on the results of individual tests run as part of the cloud mask, an algorithm was developed to estimate the phase of the clouds (liquid water, ice, or undetermined phase). The cloud optical thickness and effective radius were derived for both liquid water and ice clouds that were detected during each flight, using a nearly identical algorithm to that implemented operationally to process MODIS cloud data from the Aqua and Terra satellites (Collection 5). This analysis shows that the cloud mask developed for operational use on MODIS, and tested using MAS and MASTER data in TC4, is quite capable of distinguishing both liquid water and ice clouds during daytime conditions over both land and ocean. The cloud optical thickness and effective radius retrievals use five distinct bands of the MAS (or MASTER), and these results were compared with nearly simultaneous retrievals of marine liquid water clouds from MODIS on the Terra spacecraft. Finally, this MODIS‐based algorithm was adapted to Multiangle Imaging SpectroRadiometer (MISR) data to infer the cloud optical thickness of liquid water clouds from MISR. Results of this analysis are compared and contrasted.