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Urbanization presents significant challenges to air quality and climate resilience, necessitating pioneering urban design solutions to enhance air circulation and mitigate pollutants. This urgency intensifies in densely populated and rapidly evolving regions like Wuhan, China, where effective strategies are crucial for sustainable development. This study introduces an innovative 3D Urban Form Optimization (3D-UFO) methodology aimed at advancing urban block design configurations to improve urbanization quality. The 3D-UFO approach systematically addresses the multifaceted challenges of climate change and air quality degradation in rapidly urbanizing areas. Integrating GIS-based analysis for comprehensive Land-Use and Land-Cover Change (LULCC) evaluation with Computational Fluid Dynamics (CFD), our approach employs systematic exploration guided by established urban airflow study protocols. Robust metrics—Airspeed-Ratio (ASR) and Average-Age-of-Local-Air (ALA)—quantify the impact of diverse urban block design strategies on air-circulation efficiency and pollutant dispersion. Analysis across various urban scenarios, yielded by the proposed 3D-UFO approach, reveal significant variations in air-circulation efficiency at street and building levels (SBLs). Optimal urban air circulation achieves efficiency levels of 50–70 % when airflow aligns orthogonally across and parallel to streets. Adjusting street-level building heights, especially incorporating taller structures, boosts ventilation efficiency by 20–30 %, which is crucial for improving airflow dynamics in urban settings. Higher Height-to-Width (H/W) ratios (>5.5) yield a 218.5 % increase in ventilation in specific urban layouts. Notably, the synergy of street-aspect-ratio and building-height-ratio adjustments significantly enhance ASR and ALA, providing a quantitative foundation for sustainable urban development. This 3D-UFO methodology, fusing LULCC analysis, CFD simulations, and systematic exploration, emerge as a valuable framework for urban planners and designers. The study offers informed insights into urban sustainability challenges, demonstrating advancements in addressing environmental concerns and improving living conditions within densely populated environments.