Plants provide many ecosystem services in urban environments, including improving ambient air quality. Leaves of plants permit the deposition of particulate matter (PM) and, depending on their leaf traits, PM may be immobilized within the epicuticular wax (EW) layer, on trichomes, on hyphae of fungi, or inside stomatal cavities. In this study, leaves of 96 perennial urban plant species consisting of 45 deciduous broadleaf/needle-like trees, 32 deciduous broadleaf shrubs, 12 evergreen needle/scale-like trees, 5 evergreen broadleaf trees, and 2 climber species were investigated in June and September 2016 to determine the effectiveness of distinct leaf surfaces in PM immobilization after leaf washing treatment. The leaf surfaces were washed vigorously using a vortex shaker. The magnetizable component of accumulated and immobilized PM on the leaf surfaces was estimated using saturation isothermal remanent magnetization (SIRM) of the unwashed and washed leaves, respectively. In June, the washed leaf SIRM of deciduous (broadleaf/needle-like) tree and shrub species (n = 77) ranged between 0.1 and 13.9 μA. In September, the washed leaf SIRM of all investigated plant species (n = 96) ranged between 1.2 and 35.0 μA. Outcomes of this study indicate that leaves of Buddleja davidii, Viburnum lantana, and Sorbus intermedia showed the highest washed leaf SIRM and thus were the most effective in immobilizing PM on their leaf surfaces while leaves of Populus alba, Robinia pseudoacacia, and Abies fraseri with lowest washed leaf SIRM were the least effective. On average, more than half (i.e., 60%) of the magnetic signal still remained after vigorous washing but a large variation exists between species (9–96%). The leaf SIRM of washed leaves of deciduous broadleaf tree and shrub species was significantly higher compared to leaves of evergreen needle/scale-like species. Evidently, the magnetic signal of unwashed leaves was higher than washed ones and higher in September than in June. Leaf traits significantly influenced the magnetic signal of both washed and unwashed leaves: leaves with a high trichome density or high leaf wettability showed a higher unwashed and washed leaf SIRM compared to leaves with no trichomes or low leaf wettability. The effect of epicuticular wax structure types on leaf SIRM was indicated to be only marginally significant. Moreover, also the immobilized fraction of PM was significantly affected by trichome density and leaf wettability, thus substantiating that plant species with high trichome density and/or leaf wettability not only accumulate more PM but are also less prone to PM re-suspension than other species. In general, the results also indicate that leaf SIRM of unwashed leaves can be a good indicator to determine the effectiveness of a plant species in PM immobilization. Plant species effective in immobilizing PM on their leaf surfaces may likely improve ambient air quality when planted in urban environments. However, it is vital that leaves of these plant species (i.e., with high PM immobilization abilities) are carefully recycled as they may be polluted.