The study reports on the atmospheric concentrations of per- and polyfluoroalkyl substances (PFAS) and volatile methyl siloxanes (VMS) measured using sorbent-impregnated polyurethane foam disks (SIPs) passive air samplers. New results are reported for samples collected in 2017, which extends temporal trend information to the period 2009–2017, for 21 sites where SIPs have been deployed since 2009. Among neutral PFAS, fluorotelomer alcohols (FTOHs) had higher concentrations than perfluoroalkane sulfonamides (FOSAs) and perfluoroalkane sulfonamido ethanols (FOSEs) with levels of ND‒228, ND‒15.8, ND‒10.4 pg/m3, respectively. Among ionizable PFAS, the sum of perfluoroalkyl carboxylic acids (PFCAs) and perfluoroalkyl sulfonic acids (PFSAs) in air were 0.128–781 and 6.85–124 pg/m3, respectively. Longer-chain i.e. C9–C14 PFAS, which are relevant to the recent proposal by Canada for a listing of long-chain (C9–C21) PFCAs to the Stockholm Convention, were also detected in the environment at all site categories including Arctic sites. Cyclic and linear VMS ranged between 1.34‒452 and 0.01–12.1 ng/m3, respectively, showing dominance in urban areas. Despite the wide range of levels observed across different site categories, geometric means of the PFAS and VMS groups were fairly similar when grouped according to the five United Nations regions. Variable temporal trends in air (2009–2017) were observed for both PFAS and VMS. PFOS, which has been listed in the Stockholm Convention since 2009, is still showing increasing tendencies at several sites, indicating constant input from direct and/or indirect sources. These new data inform international chemicals management for PFAS and VMS. Display omitted •First global scale assessment (41 sites) of PFAS and VMS in air from a single program.•Long-chain PFAS were also detected globally in the environment including the Arctic.•Several ionizable PFAS, including PFOS, PFOA and PFHxS, showed increasing trends.•Neutral PFAS and VMS generally showed stable or declining levels.