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In this study, a retrospective analysis of the relationship between the land use/land cover (LULC) change and associated surface urban heat island (SUHI) effect in fast-growing Greater Hefei between 1995 and 2016 was performed. Our results reveal the heterogeneous patterns of LULC change. The concentric buffer-based urban–rural gradient analysis reveals that most of the newly emerging developed land occurred within downtown Hefei. In contrast, in three suburban municipality/county jurisdictions, the overall area change in the non-developed land was much lower, but the net increase in developed land is remarkable. Meanwhile, the spatiotemporal patterns of SUHI are in good agreement with that of the developed land, as evidenced by the notable increase in SUHI intensity (SUHII) levels and SUHI spatial extent (SUHISE) in response to the rapid urban expansion, particularly along transportation corridors. In addition, partial least square regression (PLSR) models indicate that the buffer-based predictors/independent variables are significantly related to the responses (SUHII and SUHISE), explaining approximately 61.3% of the variance in the SUHII and 79.8% of the variance in the SUHISE, respectively. Furthermore, the relative strength of the independent variables in determining the relationship was quantitatively examined. The findings of this study provide clear evidence for decision making for sustainable land development and mitigation of the SUHI effect. [ABSTRACT FROM AUTHOR]