The unplanned and uncontrolled urbanization of Indian cities has put them under different ecological and environmental threats. Urban heat island (UHI) is one such critical ecological hazard, whereby an urban area is experiencing higher land surface temperature (LST) as compared to the surrounding rural area. In the present study, the relationship of LST and surface urban heat island (SUHI) with the degree of impervious surface (IS) and green spaces (GS) in four rapidly growing Indian cities is presented. This study utilizes different geospatial techniques, including urban-rural gradient analysis, surface urban heat island estimation using Landsat OLI/TIRS data. The results signify a strong negative correlation of LST with the IS for Ahmedabad, Jodhpur, and Nagpur, while a positive correlation is seen over Guwahati. The negative correlation is the manifestation of the urban cool island, pertaining to higher LST over rural areas. On the other hand, Guwahati is surrounded by green vegetation, which provides natural cooling and thus lowers the LST, resulting in positive SUHI. The density of GS is found to be a significant contributor of SUHI in Guwahati city, whereas in the other three cities, its impact is insignificant due to its presence in very less amount in rural surroundings.