Urbanization and industrialization have escalated air pollution into a critical global issue, particularly in urban areas. Urban green infrastructures (GIs), such as parks and street trees, play a vital role in mitigating air pollution through dry deposition, the process by which air pollutants are removed by deposition onto plant surfaces or through plant uptake. However, existing studies on the dry-deposition capacity of urban green spaces are limited in their ability to reflect variations at the tree-species level, hindering comprehensive evaluations and effective management strategies. This study aims to quantitatively assess the dry-deposition capacity of the urban green spaces of Beijing and Shanghai for six major air pollutants in using an improved dry-deposition model and tree-species-specific data. Results showed that Shanghai’s urban green spaces had a monthly average dry-deposition rate of 5.5 × 10−6 s m−1, slightly higher than Beijing’s rate of 5.3 × 10−6 s m−1. Significant seasonal variations were observed, with summer showing the highest deposition rates due to favorable meteorological conditions. Broad-leaved species such as Zelkova serrata in Beijing and Photinia serratifolia in Shanghai exhibited superior dry-deposition capacities compared to coniferous species. Temperature significantly influenced dry-deposition rates for gaseous pollutants, while particulate-matter deposition was primarily affected by pollutant concentrations. This study provides critical insights into the air = purification functions of urban green spaces and underscores the importance of species selection and strategic green-space planning in urban air-quality management, informing the development of optimized urban-greening strategies for improved air quality and public health.