This study aims to investigate the mechanisms and health risks of fluoride enrichment in groundwater in the Loess Plateau, China. By taking Dali County, Shaanxi Province, China as an example, this study obtains the following results through field investigation and the analyses of water, soil, and crop samples. (1) The groundwater can be divided into two major types, namely the Quaternary pore-fissure water and Karst water. The Karst area and sandy area have high-quality groundwater and serve as the target areas for optional water supply. The groundwater in the study area is slightly alkaline and highly saline. Meanwhile, high-fluoride groundwater is mainly distributed in the loess and river alluvial plains in the depression area of the Guanzhong Basin and the discharge areas of the groundwater, with the highest fluoride concentration exceeding seven times the national standard. (2) Fluoride in groundwater mainly originates from a natural source and human activities. The natural source refers to the fluoride-bearing minerals in rocks and soil, and the fluoride from this source is mainly controlled by natural factors such as climate, geologic setting, pH, specific hydrochemical environment, ion exchange, and mineral saturation. Human activities in modern life can be further divided into industrial and agricultural sources primarily. (3) The health risks of fluoride contamination are very high in the Loess Plateau, especially for children compared to adults. Meanwhile, the risks of fluoride exposure through food intake are higher than those through drinking water intake. The authors suggest selecting target areas to improve water supply and ensure the safety of drinking water in the study area. Besides, it is necessary to plant crops with low fluoride content or cash crops and to conduct groundwater treatment to reduce the fluoride concentration in drinking water. These results will provide a theoretical basis for safe water supply in the faulted basin areas in the Loess Plateau.