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The radiances scattered or emitted by clouds demonstrate diverse features at different wavelengths due to different cloud physical structures. This paper presents a method (the smallest-radiance-distance method, SRaDM) of revealing the physical structures of clouds. The method is based on multi-spectral radiances measured by the Moderate Resolution Imaging Spectroradiometer (MODIS) onboard Aqua. The principle and methodology of SRaDM is deduced and provided in this paper. Correlation analysis based on data from MODIS and Cloud Profiling Radar (onboard CloudSat), collected from January 2007 to December 2010 over an ocean area (15°N–45°N, 145°E–165°E), led to selection of radiances at 13 wavebands of MODIS that demonstrated high sensitivity to cloud physical structures; radiances at the selected wavebands were subjected to SRaDM. The Standardized Euclidean distance is introduced to quantify the degree of changes in multi-spectral radiances (termed Drd) and in physical structures (termed Dst) between cloud profiles. Statistics based on numerous cloud profiles show that Drd decreases monotonically with a decrease in Dst, which implies that small Drd always accompanies small Dst. According to the law of Drd and Dst, the new method, SRaDM, for revealing physical structures of clouds from the collocation of cloud profiles of similar multi-spectral radiances, is presented. Then, two successful experiments are presented in which cloud physical structures are captured using multi-spectral radiances. SRaDM provides a way to obtain knowledge of the physical structures of clouds over relatively larger areas, and is a new approach to obtaining 3D cloud fields.