Plants play a vital role in mitigating aerosol particles and improving air quality. This study investigated the composition characteristics and potential effects of particles retained on the leaf surfaces of two amphibious plants (i.e., Alternanthera philoxeroides and Hydrocotyle vulgaris) in both terrestrial and aquatic habitats. The results show that plant habitats influenced the composition of aerosol particles retained on leaf surfaces. Specifically, plants in terrestrial habitats retained a higher mass concentration of coarse and large particles rich in inorganic Ca2+, accounting for over 70% of total ions, whereas plants in aquatic habitats retained a greater abundance of fine and secondary particles with high fractions of water-soluble NO3− and SO42−, taking up over 65% of total anions. Secondary particles deposited on the surfaces of plants in aquatic habitats tend to deliquesce and transform from the particle phase to the liquid phase. Terrestrial habitats facilitate the deposition of large particles. Additionally, particle accumulation on leaf surfaces adversely affected the stomatal conductance of plant leaves, leading to reductions in both the transpiration and photosynthetic rates. This study provides insights into the impact and role of plants from different habitats in mitigating urban particulate pollution.