Urban expansion intensifies population exposures to fine particulate matter (PM2.5). Trees mitigate pollution by dry deposition, in which particles settle on plants. However, city-scale models frequently overlook differences in tree species and structure. This study assesses PM2.5 removal by individual city-owned street trees in Mississauga, Canada, throughout the 2019 leaf-growing season (May to September). Using a modified i-Tree Eco framework, we evaluated the removal of PM2.5 by 200,560 city-owned street trees (245 species) in Mississauga from May to September 2019. The model used species-specific deposition velocities (Vd) from the literature or leaf morphology estimates, adjusted for local winds, a 3 m-resolution satellite-derived Leaf Area Index (LAI), field-validated, crown area modelled from diameter at breast height, and 1 km2 resolution PM2.5 data geolocated to individual trees. About twenty-eight tons of PM2.5 were removed from 200,560 city-owned trees (245 species). Coniferous species (14.37% of trees) removed 25.62 tons (92% of total), much higher than deciduous species (85.63%, 2.18 tons). Picea pungens (18.33 tons, 66%), Pinus nigra (3.29 tons, 12%), and Picea abies (1.50 tons, 5%) are three key species. Conifers’ removal efficiency originates from the faster deposition velocities, larger tree size, and dense foliage, all of which enhance particle deposition. This study emphasizes species-specific approaches for improving urban air quality through targeted tree planting. Prioritizing coniferous species such as spruce and pine can improve pollution mitigation, providing actionable strategies for Mississauga and other cities worldwide to develop green infrastructure planning for air pollution.