To learn the extent of human exposure to polyfluoroalkyl compounds (PFCs) in a remote fishing population, we measured, in Faroese children and pregnant women, the serum concentrations of nine PFCs, including perfluorooctane sulfonate (PFOS), perfluorooctanoate (PFOA), and perfluorononanoate (PFNA), by using online solid-phase extraction coupled to isotope dilution high-performance liquid chromatography-tandem mass spectrometry. The serum samples analyzed had been collected between 1993 and 2005 from 103 children 7 years of age, 79 of these children at 14 years of age, and from 12 pregnant women and their children 5 years later. PFOS was detected in all samples analyzed, and both PFOA and PFNA were detected in all but one of the samples. The concentrations found are comparable tothose reported elsewhere. Correlations between paired concentrations were poor. However, PFOS and PFNA concentrations correlated well with the frequency of pilotwhale dinners and with concentrations of mercury and polychlorinated biphenyls. One whale meal every two weeks increased the PFOS concentration in 14-year-olds by about 25% and PFNA by 50%. The high frequency of detection of most PFCs suggests widespread exposure in the Faroe Islands already by the early 1990s, with whale meat being an important source.