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Antimony pollution in the groundwater of the Xikuangshan (XKS) antimony (Sb) mine area in China's Hunan Province has attracted increasing attention. A total of 43 water samples were collected to help understand the hydrogeochemical characteristics, identify the Sb source, and evaluate the water–rock interactions of the Shetianqiao aquifer (SA). The Sb concentrations in shallow and deep SA water samples were 0.1–47.4 mg L−1 and 0.3–19.2 mg L−1, respectively. Stibnite oxidation and leaching from arsenic alkali residue mine wastes were the main Sb sources for the shallow SA water, whereas stibnite oxidation and stronger water–rock interaction were the predominant Sb sources for the deep SA water. The higher Sb concentration (> 10.0 mg L−1) in shallow SA water was predominantly induced by weathering of Sb-bearing minerals, evaporation/concentration effects, and cation exchange, whereas the higher Sb concentration in deep SA water was largely caused by weathering of Sb-bearing minerals, evaporation/concentration effects, ion exchange, and competitive adsorption. These findings provide a more detailed understanding of the geochemical behavior of Sb in groundwater and can be used to develop suitable Sb pollution management strategies. [ABSTRACT FROM AUTHOR]