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The present work investigated the composition evolution of the TMS series of Ni-base single crystal (SC) superalloys in light of the cluster formula approach systematically. The cluster formula of SC superalloys could be expressed with [Formula see text], in which all the alloying elements were classified into three groups, Al series ([Formula see text]), Cr series ([Formula see text]), and Ni series ([Formula see text]). It was found that the total atom number (Z) of the cluster formula units for TMS series of superalloys varies from Z