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With rapid urbanization and industrialization, PM2.5 pollution exerts a significant negative impact on the urban eco-environment and on residents’ health. Previous studies have demonstrated that cities in China are characterized by urban particulate matter island (UPI) phenomena, i.e., higher PM2.5 concentrations are observed in urban areas than in rural settings. How, though, nature and socioeconomic environments interact to influence UPI intensities is a question that still awaits a general explanation. To fill this knowledge gap, this study investigates spatiotemporal variations in UPI effects with respect to different climatic settings and city sizes in 240 cities in China from 2000 to 2015 using remotely sensed data and explores the effective mechanism of human–environmental factors on UPI dynamics based upon the Geographically Weighted Regression (GWR) model. In particular, a conceptual framework that considers natural environments, technology, population, and economics is proposed to explore the factors influencing UPIs. The results show (1) that about 70% of the cities in China selected exhibited UPI effects from 2000 to 2015. In addition, UPI intensities and the number of UPI-related cities decreased over time. It is noteworthy that PM2.5 pollution shifted from urban to rural areas. (2) Elevation was the most efficient driving factor of UPI variations, followed by precipitation, population density, NDVI, per capita GDP, and PM2.5 emission per unit GDP. (3) Climatic backgrounds and city sizes influenced the compositions and performance of dominant factors regarding UPI phenomena. This study provides valuable a reference for PM2.5 pollution mitigation in cities experiencing global climate change and rapid urbanization and thus can help sustainable urban developments.

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