Cities are responsible for more than 80% of global greenhouse gas emissions. Sequestration of air pollutants is one of the main ecosystem services that urban forests provide to the citizens. The atmospheric concentration of several pollutants such as carbon dioxide (CO2), tropospheric ozone (O3), and particulate matter (PM) can be reduced by urban trees through processes of adsorption and deposition. We predict the quantity of CO2, O3, and PM removed by urban tree species with the multilayer canopy model AIRTREE in two representative urban parks in Italy: Park of Castel di Guido, a 3673 ha reforested area located northwest of Rome, and Park of Valentino, a 42 ha urban park in downtown Turin. We estimated a total annual removal of 1005 and 500 kg of carbon per hectare, 8.1 and 1.42 kg of ozone per hectare, and 8.4 and 8 kg of PM10 per hectare. We highlighted differences in pollutant sequestration between urban areas and between species, shedding light on the importance to perform extensive in situ measurements and modeling analysis of tree characteristics to provide realistic estimates of urban parks to deliver ecosystem services.