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This study utilizes high-resolution population grid data from 2004 to 2018 to assess the extent of urban polycentricity in 284 Chinese prefecture-level cities. A new method for measuring urban polycentricity is devised using the Clauset-Newman-Moore grey modularity maximization algorithm. Additionally, the Spatial Durbin Model is applied to investigate the effect of urban polycentricity on the mean and spatial variation of PM 2.5 concentrations. Our statistical results show that the increased distance between urban centers and the increased size disparity between the large and small centers effectively reduces air pollution within the city. On the other hand, in cities with a strong clustering of urban centers and significant size disparity between main and sub-centers, the polycentric urban structure cannot help reduce air pollution but merely shift it to other urban centers within the city. Hence, interpreting the severity of urban air pollution solely on the basis of the citywide average of air pollution may be insufficient. It is necessary to consider the possible relocation of air-polluting activities associated with polycentric urban structures. Policymakers should take into account the potential spatial inequality of air pollution driven by urban polycentricity. [Display omitted] • New algorithm for measuring urban polycentricity (distance dispersion and size disparity of urban centers). • New approach for measuring "urban" air pollution. • Suggested method for addressing the spatial spillover effects of air pollution in data analysis. • Polycentric urban structures reduce air pollution but exacerbate the uneven distribution of air pollution. • Benefits and potential drawbacks of urban polycentricity in mitigating air pollution. [ABSTRACT FROM AUTHOR]