The datasets presented here are related to the research paper entitled “Disordered Gd6UO12-δ with the cation antisite defects prepared by a combined mechanochemical−thermal method” [1]. The datasets complement the findings [1] on the effect of the combined mechanochemical−thermal processing of the stoichiometric mixture of solid pre cursors (3Gd2O3 + UO2) on the formation of Gd6UO12-δ phase. In this article, we provide (i) X-ray diffraction (XRD) data of the 3Gd2O3 + UO2 mixture milled for 12 h, (ii) the refined XRD data of the non-milled 3Gd2O3 + UO2 mixture after annealing at 1282 °C for 3 h in air, and (iii) the thermogravimetric and differential thermal analysis (TG-DTA) data for non-milled and mechanically preactivated3Gd2O3+UO2 mixturemeasuredinairataheatrateof 10K/min.