Cross-country assessment of aerosol loading was made over several South Asian megacities using multiple high-resolution remote-sensing database to assess how aerosols vary within the city and its suburbs. Parameters sensitive to aerosol optical and microphysical properties were processed over city-core and its surrounding, separated by a buffer. Cities across the Indo-Gangetic Plain (IGP; AOD:0.52–0.72) along with Mumbai (0.47) and Bangalore (0.46) denote comparatively high aerosol loading against non-IGP cities. City-core specific AOD was invariably high compared to surrounding, however with varying gradient having robust geographical signature. Exceptions to this general trend were in Kathmandu (ΔAOD: 0.07) and Dhaka (ΔAOD: 0.01) while strong positive AOD gradient was noted in Bangalore (+0.11), Colombo (+0.08) and in Mumbai (+0.07). While all mainland cities exhibited robust intraannual variability, distinction between city-core and its surrounding AOD exhibited varying seasonality. City-specific geometric coefficient of variation indicated insignificant association with mean AOD as opposed to European and American cities. Both pixel-based and city-specific analysis revealed a strong increasing trend in AOD with highest magnitude in Varanasi and Bangalore. Aerosol sub-types based on aerosols’ sensitivity to UV-absorption and particle size denotes higher relative abundance of carbonaceous smoke aerosols within city-core, without having significant distinction for mineral dusts and urban aerosols.