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The data presented in this article relate to the research article entitled "Superior room-temperature power factor in GeTe systems via multiple valence band convergence to a narrow energy range" [T. Oku et al., Mater. Today Phys. 20 (2021) 100484 (10.1016/j.mtphys.2021.100484)]. Polycrystalline (GeTe) n Sb2Te3 (n = 10, 12, 16, 20, and 24) bulk samples were prepared by melting and annealing. The Ge defect concentration of each composition was estimated from Rietveld refinement of the synchrotron X-ray powder diffraction patterns. Elect