China's unprecedented rapid urbanization has dramatically reshaped the urban built environment, disrupting the thermal balance of cities. This disruption causes the urban heat island (UHI) effect, adversely affecting urban sustainability and public health. Although studies have highlighted the remarkable impacts of the built environment on UHIs, the specific effects of its various structures and components remain unclear. In this study, a multidimensional remote sensing data set was used to quantify the atmospheric UHIs across 335 Chinese cities from 1980 to 2020. In conjunction with stocks of three end-use sectors and three material groups, the impacts of gridded material stocks on UHI variations were analyzed. The findings reveal that building stocks exert a predominant influence in 48% of cities. Additionally, the extensive use of metal and inorganic materials has increased thermal stress in 220 cities, leading to an average UHI increase of 0.54 °C. The effect of organic materials, primarily arising from mobile heat sources, is continuously increasing. Overall, this study elucidates the effect of the functional structure and material composition of urban landscapes on UHIs, highlighting the complexities associated with the influence of the built environment on the urban heat load.