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Urban trees provide important ecosystem services, including air quality improvement. Polycyclic aromatic hydrocarbons (PAHs) are among the most important pollutants in air, due to their elevated concentrations and toxicity. Plants can act as filters of PAHs and as "chemical reactors" for pollutant removal, therefore reducing air concentrations. Here, the first assessment of photo- vs. biodegradation of PAHs on leaves of urban trees is presented. A dynamic air-vegetation-soil model (SoilPlusVeg) was improved to simulate the fate of two representative PAHs with contrasting physico-chemical properties (phenanthrene and benzo[a]pyrene). Simulations were performed for two different environmental scenarios from Italy (Como and Naples), selected for their dissimilar meteorological parameters, plant species and emission levels. The effect of photo- and biodegradation on leaf concentrations and fluxes towards air and soil was investigated comparing deciduous (maple, cornel and hazelnut) and evergreen (holm oak) broadleaf woods. The results showed that biodegradation in the phyllosphere could not be neglected when evaluating the ecosystem services provided by urban trees, as this process contributed significantly to the reductions (up to 25% on average) in PAH leaf concentrations and fluxes to air and soil; however, the reductions revealed ample variations with time (up to more than two orders of magnitude) showing the dependence on meteorological parameters, air compartment structure, as well as type of woods. These findings permitted to improve the ecological realism of the simulations and obtain more accurate results when predicting organic contaminant uptake and release by plant leaves, including potential for food chain transfer and long-range transport., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2020 Elsevier B.V. All rights reserved.)