Air pollution remains a critical concern in rapidly urbanizing cities, where accelerated development and the uneven distribution and limited accessibility of green spaces exacerbate environmental challenges. Although urban green spaces can mitigate pollution, their effectiveness is often constrained by inadequate planning and management strategies. To address these issues, this study proposes a multi-stage, scenario-driven green space optimization framework that applies data-driven modeling approaches to spatially assess and maximize pollutant-specific air quality benefits. The proposed methodology integrates remote sensing data, classification algorithms, vegetation indices, and hyperspectral and bioclimatic indicators to assess canopy health, structural characteristics, and guide species-level tree selection. Additionally, a GIS-based decision support system was developed to enable real-time, adaptive urban planning using sensor-linked air quality data. To validate the framework, a comprehensive case study was conducted in Hangzhou, China from 2014 to 2024, evaluating air quality, vegetation health, and key environmental drivers to promote sustainable urban development. The results demonstrated significant reductions in CO, PM2.5, PM10, NO2, and SO2 across most regions, while a slight increase in O3 was observed, highlighting the complex dynamics of secondary pollutants. The Random Forest–based optimisation framework reveals a nonlinear response of pollutant concentrations to NDVI–LAI enhancement, with PM2.5 and PM10 showing the most spatially coherent reductions under +10–20 % greening, while gaseous pollutants exhibit weaker, spatially heterogeneous responses; temporal quadrant analysis further indicates sustained-improvement dominance for NO2 and SO2, contrasted by greater instability and trade-off behaviour for O3 and PM10. The novelty of this study lies in introducing an AI-based optimization framework that leverages machine learning and spatial–temporal diagnostics to identify where and how urban green spaces can most effectively reduce different air pollutants, offering a practical decision-support approach beyond traditional correlation analyses. Future research should emphasize practical implementation by incorporating socioeconomic, health, and accessibility metrics to support the development of sustainable cities and a climate-resilient society.
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