Nature-based solutions have been identified by the European Union as being critical for the enhancement of environmental qualities in cities, where urban and peri-urban forests play a key role in air quality amelioration through pollutant removal. A remote sensing and geographic information system (GIS) approach was applied to the Metropolitan City (MC) of Rome to assess the seasonal particulate matter (PM10) removal capacity of evergreen (broadleaves and conifers) and deciduous species. Moreover, a monetary evaluation of PM10 removal was performed on the basis of pollution externalities calculated for Europe. Deciduous broadleaves represent the most abundant tree functional group and also yielded the highest total annual PM10 deposition values (1769 Mg). By contrast, PM10 removal efficiency (Mg·ha−1) was 15%–22% higher in evergreen than in deciduous species. To assess the different removal capacity of the three functional groups in an area with homogeneous environmental conditions, a study case was performed in a peri-urban forest protected natural reserve (Castelporziano Presidential Estate). This study case highlighted the importance of deciduous species in summer and of evergreen communities as regards the annual PM10 removal balance. The monetary evaluation indicated that the overall PM10 removal value of the MC of Rome amounted to 161.78 million Euros. Our study lends further support to the crucial role played by nature-based solutions for human well-being in urban areas.