The relationship between the land cover (LC) characteristics and the land surface temperature (LST) is significant for surface urban heat island (SUHI) study and for sustainability research. To better understand how the land surface temperature (LST) responds to LC, two urban areas, Vienna and Madrid, with different climatic conditions are selected and compared, using Landsat-8 OLI data and urban atlas data. To determine a suitable scale for analyzing the relationship between LC and LST, a correlation analysis at different sizes of spatial analytical scales is applied. To demonstrate the LC composition effects on LST, a regression analysis of the whole study area and in the specific circumstance is undertaken. The results show that: (1) In the summer, Vienna presents high temperature in the urban areas and low temperature in the surrounding rural areas, while Madrid displays the opposite appearance, being relatively cooler in the urban areas as compared to the rural areas, with the main different factors affecting elevated urban LST; (2) Suitable analytical scales are suggested in studying the LC-LST relationship between different LC characteristics in the two study areas; (3) Negative effects on the LST appear when the area of cooling sources, such as water or urban greenery, reaches 10% at a 990 × 990 m 2 scale in Vienna. Built-up area is the main factor affecting elevated urban LST where such areas cover the majority at a 990 × 990 m 2 scale in Madrid. These findings provide a valuable view regarding how to balance the urban surface thermal environment through urban planning.

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