It is of significance to elucidate the groundwater quality and hydrogeochemical processes for sustainable utilization of groundwater resources in water shortage regions. A total of 256 groundwater samples were collected in typical watersheds in Zhangjiakou, northern China. The hydrochemical parameters, conventional ions, and trace elements were measured, and ?D and ?¹⁸O data were collected to delineate the groundwater quality and hydrogeochemical processes. The results showed that 32.91% of the groundwater could be directly used for drinking water sources in the Bashang Plateau, north of the study area. The F^– and NO₃^–-N were the main parameters above the standard threshold for drinking water. In contrast, the groundwater quality in the Baxia River Basins, south of the study area, was of a better scenario. Nonetheless, high concentrations of F^–, total hardness, and SO₄^2- were still observed. Most samples in the Bashang Plateau had relatively higher salinity than the Baxia River Basins. Both surface water and groundwater in the study area originated from local meteoric water with considerable hydraulic connections. The high-fluoride groundwater was primarily formed by dissolution of fluoride-rich minerals under conditions of high pH and Na⁺, low Ca²⁺, and rich in HCO₃^–. The dissolution of carbonate and silicate minerals accompanied by strong cation exchange and weak evaporation was the dominant water-rock interaction affecting the hydrochemical composition of groundwater, and anthropogenic NO₃^– input had an extra influence on hydrochemical process. This study provides a scientific guideline for the protection and allocation of local groundwater resources.