In this study, the concentration of fluoride and the associated health risks for infants, children, and adults were analyzed and compared for three drinking water sources in Yancheng City, Jiangsu Province, China. To analyze the relationship between the water quality parameters of pH, fluoride (F−), sulfate (SO42−), chloride (Cl−), total dissolved solids (TDS), total alkalinity (TAlk), sodium (Na+), and potassium (K+), statistical analyses including correlation analysis, R-mode cluster analysis and factor analysis were performed based on monthly data from the year 2010 to 2015. The results indicated: (1) Fluoride concentrations in the drinking water sources ranged from 0.38 to 1.00 mg L−1 (mean = 0.57 mg L−1) following the order of Tongyu River > Yanlong Lake > Mangshe River; (2) fluoride concentrations in 22.93% of the collected samples were lower than 0.5 mg L−1, which has the risk of tooth cavities, especially for the Mangshe River; (3) the fluoride exposure levels of infants were higher than children and adults, and 3.2% of the fluoride exposure levels of infants were higher than the recommended toxicity reference value of 122 μg kg−1 d−1 as referenced by Health Canada, which might cause dental fluorosis issues; (4) the physico-chemical characteristics are classified the into four groups reflecting F−- TAlk, Na+-K+, SO42−-Cl−, and pH-TDS, respectively, indicating that fluoride solubility in drinking water is TAlk dependent, which is also verified by R-mode cluster analysis and factor analysis. The results obtained supply useful information for the health department in Yancheng City, encouraging them to pay more attention to fluoride concentration and TAlk in drinking water sources.