Drinking water contamination by perfluoroalkyl and polyfluoroalkyl substances (PFASs) is an issue of relatively recent concern. The literature indicates that anion exchange resins and granular activated carbon (GAC) are suitable technologies for removing these compounds. While several laboratory-scale and pilot-scale experiments have been conducted to study activated carbon adsorption/desorption mechanisms of a number of PFASs, little data on full-scale plants are available. This work examines a real case of groundwater contamination by PFASs in an area of approximately 200 km2. The performance of the main drinking water treatment plant in the area (flowrate = 30,000 m3/d; 100,000 people served), which is equipped with GAC filters, was analysed. Approximately 17,000 analytical data points from a working period of five years were processed. Perfluorobutyric acid (PFBA) was the first compound to attain breakthrough, followed by perfluoropentanoic acid, perfluorohexanoic acid, perfluorobutanesulfonic acid, and perfluorooctanoic acid (PFOA). The adsorption capacity and treated bed volumes at complete breakthrough (saturation) were calculated, and ranged from 1.71 g/t and 7100 (PFBA) to 24.6 g/t and 50,900 (PFOA), with the total organic carbon concentration in the groundwater ranging from <0.1 to 0.5 mg/L. The overall adsorption capacity was approximately 40 g of total PFASs/t. The breakthrough behaviour of PFASs was correlated with the CF chain length, the type of hydrophilic head (either carboxyl or sulfonic), and the n-octanol/water partition coefficients logP and logD. The results corroborate the findings of previously published bench-scale and pilot-scale experiments.