The contamination status of perfluoroalkyl substances (PFASs) were investigated in 64 tapwater samples collected from 17 cities and 45 surface water samples from adjacent areas in the eastern China. The total PFAS concentrations in tapwater ranged from 1.4 to 175 ng/L; relatively higher PFAS levels were observed in samples collected from the Yangtze River Delta region, which was similar to the geographical distribution pattern of PFAS levels observed in rivers and lakes. The highest total PFASs in tapwater was found in Changshu, where several fluorine-related industries are located, whereas the lowest was observed in Beijing. Significant positive correlations between PFAS compositions in tap water sample and their source waters were noted. Several industries such as paper, textile, and leather industries may contribute to the contamination of PFASs in tapwater.