Feathers have been shown to be useful in the biomonitoring of environmental contaminants, such as metals and persistent organic pollutants. However, little is known regarding the levels of perfluoroalkyl acids (PFAAs) in feathers and the applicability of these structures for the biomonitoring of these compounds. In the present study, we report the extent to which feathers are suitable for monitoring PFAA concentrations in the blood plasma of an insectivorous songbird model species, the great tit (Parus major), settled at and in the vicinity of a fluorochemical plant in Antwerp, Belgium. For most of the target analytes (out of the 15 investigated), the feather PFAA concentrations near the plant are the highest ever reported in free-living birds. As PFAA concentrations did not differ in the adjacent sites, no pollution gradient with distance from the plant was observed. In addition, the PFAA concentrations were not associated with the age and sex of the birds. Perfluorooctanoic acid (PFOA) concentrations were significantly higher in P. major feathers than in blood plasma, but for most other PFAAs, these differences were not observed. The concentrations of perfluorooctanesulfonate (PFOS) and PFOA in P. major feathers and plasma were significantly and positively correlated when combining data from all sites but often not at individual sites. This result was likely caused by lower sample sizes at the individual sites and the use of matrices that represent different time periods. Our results suggest that P. major feathers cannot be used to estimate PFOA and PFOS concentrations in blood plasma, except when there is a great deal of variation in pollutant concentrations among sites/individual birds. Both matrices represent different time frames, providing complementary information on environmental PFAA concentrations, as illustrated by the observation that more PFAA compounds could be detected in P. major feathers than in blood plasma.