A novel approach combining gas chromatography-atmospheric pressure laser ionization-time-of-flight-mass spectrometry (GC-APLI-MS) with the micrometeorological eddy covariance (EC) technique is demonstrated to quantify particle-bound polycyclic aromatic hydrocarbons (PAH) mass fluxes above a central European city. During the case study, 18 different PAH compounds could be identified in two one-hour particle samples and, in combination with size-resolved particle deposition velocities obtained from EC measurements, inferred particulate PAH mass fluxes for two respective size fractions (0.060–0.108 μm and 0.170–10 μm) were quantified. Maximum concentrations and fluxes (in the order of 0.9 ± 0.09–17 ± 8 ng m−2 hr−1) were estimated for the 5-ring PAHs benzo[e]pyrene, benzo[a]pyrene and perylene. Fingerprints of PAH concentrations suggest strong pyrogenic sources, particularly wood burning.