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In the current study area (Faridabad, Gurugram, Ghaziabad, and Gautam Buddha Nagar), the aerosol concentration is very high, adversely affecting the environmental conditions and air quality. Investigating the impact of Land Use Land Cover (LULC) on Aerosol Optical Depth (AOD) helps us to develop effective solutions for improving air quality. Hence, the spectral indices derived from LULC ((Normalized difference vegetation index (NDVI), Soil adjusted vegetation index (SAVI), Enhanced vegetation index (EVI), and Normalized difference build-up index (NDBI)) with Moderate Resolution Imaging Spectroradiometer (MODIS) Multiangle Implementation of Atmospheric Correction (MAIAC) high spatial resolution (1 km) AOD from the years 2010–2019 (less to high urbanized period) has been correlated. The current study used remote sensing and Geographical Information System (GIS) techniques to examine changes in LULC in the current study region over the ten years (2010–2019) and the relationship between LULC and AOD. A significant increase in built-up areas (12.18%) and grasslands (51.29%) was observed during 2010–2019, while cropland decreased by 4.42%. A positive correlation between NDBI and SAVI (0.35, 0.27) indicates that built-up soils play an important role in accumulating AOD in a semi-arid region. At the same time, a negative correlation between NDVI and EVI (−0.24, −0.15) indicates the removal of aerosols due to an increase in vegetation. The results indicate that SAVI can play an important role in PM2.5 modeling in semi-arid regions. Based on these findings, urban planners can improve land use management, air quality, and urban planning. [ABSTRACT FROM AUTHOR]