Environmental and human exposures to perfluoroalkyl substances (PFASs) are of emerging concern since they are persistent and bioaccumulative. The present study reports PFASs levels in human milk, infant formulas and baby food (dry cereals and pots) from the Valencian Community (Spain) in order to evaluate the infant exposure to these substances through the diet. The results show that perfluorobutanoic acid (PFBA) and perfluorooctanoic acid (PFOA) were in all the samples of the four selected matrices (except PFOA in one sample of dry cereal baby food). Perfluoroheptanoic acid (PFHpA) and perfluorodecanoic acid (PFDA) were also detected in 70% of the breast milk samples. In infant formulas, PFDA and perfluorooctanesulfonate (PFOS) were detected in 75% and 69%, respectively. In dry cereals baby food, PFBA was in 100% of the samples while PFOA and PFOS in 92%. In baby food pots, PFDA was also detected in 83% of the samples. Estimated daily intakes (EDIs) of PFOA (maximum 32.2 ng kg day) and PFOS (9.0 ng kg day) are lower than tolerable daily intakes (TDIs) established for PFOA (1500 ng kg day) and PFOS (150 ng kg day). ; This work has been supported by the Spanish Ministry of Economy and Competitiveness and the ERDF (European Regional Development Fund) through the project, GCL2015-64454-C2-1-R as well as by the Research Programme on Health, Prevention and Prediction of the Illness of the Regional Health Ministry of the Generalitat Valenciana (Project N° 50/2011). M. Lorenzo acknowledges the Foundation “Tatiana Pérez de Guzmán el Bueno” for the grant to get the PhD. D. Barceló acknowledges financial support from the Visiting Professor Program of the King Saud University, Riyadh, Saudi Arabia. ; Peer Reviewed