Abstract: The chambersite powders after mineral separation were prepared by 3D high-energy ball milling for 30, 40, and 50 min in this paper. Scanning electron microscope (SEM), transmission electron microscope (TEM), and X-ray diffraction (XRD) were utilized to characterize the microstructures of chambersite samples, and the Scherrer formula was used to calculate the half-height width and grain size of the samples. The luminescence properties of chambersite milled for different times were discussed. The results show that, the particle size of the chambersite samples after high-energy ball milling for 30, 40, and 50 min reaches 0.37, 0.29, and 0.28 μm, respectively. The diffraction peak of the chambersite samples is broadened with the increase of milling time, and the diffraction intensity of (202), (114), and (404) crystal faces decreases with the increases of milling time, noting the (202), (114), and (404) crystal faces are the incomplete cleavage planes. The luminescence intensity of the chamber site samples decreases remarkably with the increase of milling time.