The potential of urban greening plants to capture particulate matter (PM) from the ambient atmosphere is contingent on interactions between the level of pollution and leaf surfaces. For this study, thirteen plant species were investigated to quantify their capacity of PM accumulation under three atmospheric environments, that is, industrial, traffic and university campus (control), in Kunming City (Southwest China). The sampled sites represented different pollution levels (that is, high pollution, slight pollution and clean air, respectively). The plant species differed in their accumulation of PM by six- to eight-fold across the three sites. Magnolia grandiflora was the most efficient evergreen tree species, whereas Platanus acerifolia had the highest capture of PM among deciduous trees. The accumulation capacity of the same species varied with the degree of pollution. For example, Osmanthus fragrans, Loropetalum chinense and Cinnamomum japonicum were highly efficient for the capture of PM in the traffic and university campus areas; however, they exhibited medium accumulation in the industrial area. Prunus majestica demonstrated an intermediate accumulation capacity in the industrial area, but was low in the traffic and university campus areas. The capturing capacity of the same genus was also different among the different levels of pollution. For example, C. japonicum had a 2.9–4.2-times higher PM accumulation than did C. camphora across the three sites. There were significant differences in leaf surface area, stomata density/length, guard cell area, and trichome density/length among these species. The species-specific efficacy of PM capture was primarily contributed to by leaf size and surface roughness, stomata density, and trichome length. In particular, hairy-leaf leaves with medium stomatal density exhibited higher PM capture. Therefore, leaf micromorphology, leaf size and longevity appeared to be significant predictive factors for the accumulation of PM, which may aid in the selection of greening plant species for the remediation of pollutants in urban areas.