Due to the frequent urban air pollution episodes worldwide recently, decision-makers and government agencies are struggling for sustainable strategies to optimize urban land use/cover change (LUCC) and improve the air quality. This study, thus, aims to identify the underlying relationships between PM₁₀ concentration variations and LUCC based on the simulated PM₁₀ surfaces in 2006 and 2013 in the Changsha-Zhuzhou-Xiangtan agglomeration (CZT), using a regression modeling approach. LUCC variables and associated landscape indexes are developed and correlated with PM₁₀ concentration variations at grid level. Results reveal that the overall mean PM₁₀ concentrations in the CZT declined from 106.74 μg/m³ to 94.37 μg/m³ between 2006 and 2013. Generally, variations of PM₁₀ concentrations are positively correlated with the increasing built-up area, and negatively correlated with the increase in forests. In newly-developed built-up areas, PM₁₀ concentrations declined with the increment of the landscape shape index and the Shannon diversity index and increased with the growing Aggregation index and Contagion index. In other areas, however, the reverse happens. These results suggest that LUCC caused by urban sprawl might be an important factor for the PM₁₀ concentration variation in the CZT. The influence of the landscape pattern on PM₁₀ concentration may vary in different stages of urban development.