A novel method of determining nanocluster sizes and size distributions using high-angle annular dark-fieldimaging in scanning transmission electron microscopy is described. This method is demonstrated for MgO-supported [Os10C(CO)24]2- clusters formed by treating Os3(CO)12 precursors in CO. The image analysisidentified the presence of both Os3(CO)12 precursors and [Os10C(CO)24]2- clusters in the expected ratio (withthe sizes matching those calculated on the basis of their crystallographically determined structures within6%) and also larger clusters that can be readily identified as combinations of the former clusters.