Urbanization has caused an increase in air pollution and land surface temperature (LST) in Indian cities. This study investigated the seasonal relationship of LST with air pollutants in both cities. The relationship was examined using the LST from satellite and air pollutants data from CAAQMS. It was noted that LST has a better relationship with PM2.5 and O3 in Bengaluru and PM2.5 and NO2 in Hyderabad. In Hyderabad strong relationship has been obtained for NO2 (R2 = 0.60, p < 0.05) and CO (R2 = 0.58, p < 0.05). The interaction of LST with all air pollutants considered together was strong. The interaction in Hyderabad during summer (R2 = 0.78) and winter (R2 = 0.76), respectively, whereas it is strong during the summer season in Bengaluru (R2 = 0.62). The overall analysis indicates that the impact of individual air pollutants on LST is low to moderate. However, the combined effect of air pollutants on LST is significantly high.