Fluoride hydrogeochemistry and associated human health risks implications are investigated in several aquifers along the southern edge of the Chinese Loess Plateau. Locally, 64% shallow groundwater samples in loess aquifer exceed the fluoride limit (1.5 mg/L) with the maximum of 3.8 mg/L. Presently, the shallow groundwater is the main source of private wells for domestic use, and this is clearly a potential risk for human health. Hydrogeochemistry and stable isotopes are used to elucidate the diversity of occurrence mechanisms. Enrichment of fluoride in groundwater is largely controlled by the F-containing minerals dissolution. Furthermore, alkaline condition and calcium-removing processes promote water-rock interactions. Stable isotopes of hydrogen and oxygen (?D and ?18O) in study area waters demonstrate that groundwater in loess aquifer is old, which means groundwater remains in the aquifer for a long time. Long residence time induces sufficient water-rock interactions, which play significant roles in the resolution of fluoride minerals. Samples from the shallow loess aquifer show elevated fluoride levels, which may pose human health risk for both adults (60%) and children (94%) via oral intake. To ensure drinking water safety, management measures such as popularizing fluoride-removing techniques and optimizing water supply strategies need to be implemented.