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Optimizing urban form through urban planning and management policies can improve air quality and transition to demand-side control. Nitrogen dioxide (NO 2) in the urban atmosphere, mainly emitted by anthropogenic sources such as industry and vehicles, is a key precursor of fine particles and ozone pollution. Both NO 2 and its secondary pollutants pose health risks for humans. Here we assess the interactions between urban forms and airborne NO 2 pollution in different cities with various stages of urbanization in the Yangtze River Delta (YRD) in China, by using the machine learning and geographical regression model. The results reveal a strong correlation between urban fragmentation and tropospheric NO 2 vertical column density (TVCD) in YRD cities in 2020, particularly those with lower or higher levels of urbanization. The correlation coefficients (R2) between NO 2 TVCD and the largest patch index (a metric of urban fragmentation) in different cities are greater than 0.8. For cities at other urbanization stages, population and road density are strongly correlated with NO 2 TVCD, with an R2 larger than 0.61. This study highlights the interdependence among urbanization, urban forms, and air pollution, emphasizing the importance of customized urban landscape management strategies for mitigating urban air pollution. [Display omitted] • Effects of urban form on NO 2 changed significantly with urbanization process • Lower fragmentation reduces NO 2 pollution in lower and higher stages of urbanization • Population and road density dominate urban NO 2 pollution in middle stages of urbanization [ABSTRACT FROM AUTHOR]