Groundwater is a key medium for the migration and enrichment of elements into ore bodies in sandstone-type uranium deposits, with anomalies of uranium elements and their associated components in water serving as indicators for exploring such deposits. The Erlian Basin, located in central-northern Inner Mongolia, is a crucial production area for sandstone-type uranium deposits in China. The groundwater flow system in the basin plays a significant role in the formation of uranium deposits. To study the hydrogeochemical characteristics and enrichment regularities of groundwater uranium in the Erlian Basin, 269 groundwater samples were collected. Hydrogeochemical analysis methods, such as Piper diagrams, Gibbs diagrams, and contour maps, were employed to determine the distribution characteristics and occurrence forms of groundwater uranium in the study area. The primary water chemistry types in the study area were HCO3–Ca•Na, HCO3–Na, HCO3•SO4–Na, and SO4•HCO3–Na•Ca. The distribution range of uranium content in groundwater in the study area was 0.1–453 μg/L (average of 53.08 μg/L). A comprehensive analysis, based on the direction of groundwater flow and changes in the redox environment, suggested that the higher uranium values in groundwater were distributed in the runoff and discharge areas, with uranium anomaly points existing in areas with alternating oxidation and reduction zones. These uranium anomaly points were in good agreement with the known large uranium deposits of Nuheting, Qiharigetu, Daoersu, and others, thereby predicting six other uranium hydrochemical anomaly points as prospective areas for uranium mineralization. The pH value distribution range in the study area's groundwater was 6.8–9.1, and the redox potential (Eh) value range was -126–52 mV, indicating that uranium exists in groundwater in the form of UO2(CO3)34− and UO2(CO3)22−. An increase in bicarbonate (HCO3−) is conducive to uranium dissolution. The enrichment and occurrence forms of uranium in groundwater are influenced by the concentrations of Fe and (Ca2++Mg2+), with uranium precipitation and enrichment occurring as the groundwater evolves and changes in the redox environment. The uranium content in deep wells is higher than in nearby shallow wells, indicating that deep water circulation is beneficial for mineralization. The pH, Eh, HCO3−, Fe, and other hydrogeochemical indicators are indicative of uranium enrichment; thus, they can be considered as reference bases when exploring for potential uranium resources.