<p><strong>Abstract.</strong> Concurrent measurements of the altitude profiles of cloud condensation nuclei (CCN) concentration, as a function of supersaturation (ranging from 0.2&#8201;% to 1.0&#8201;%), and aerosol optical properties (scattering and absorption coefficients) were carried out aboard an instrumented aircraft across the Indo-Gangetic Plain (IGP) covering coastal, urban and arid environments, just prior to the onset of the Indian summer monsoon (ISM) of 2016, under the aegis of the SWAAMI - RAWEX campaign. In general, the CCN concentration has been highest in the Central IGP, decreasing spatially from east to west above the planetary boundary layer (PBL), which is ~&#8201;1.5&#8201;km for the IGP during pre-monsoon. Despite of this, the CCN activation efficiency at 0.4&#8201;% supersaturation has been, interestingly, the highest over the eastern IGP (~&#8201;72&#8201;%), followed by the west (~&#8201;61&#8201;%), and has been the least over the central IGP (~&#8201;24&#8201;%) within the PBL. In general, higher activation efficiency is noticed above the PBL than below it. The Central IGP showed remarkably low CCN activation efficiency at all the heights, which appears to be associated with high black carbon (BC) mass concentration there, indicating the role of anthropogenic sources in suppressing the CCN efficiency. First ever CCN measurements over the western IGP, encompassing &quot;The Great Indian desert&quot;, show high CCN efficiency, ~&#8201;61&#8201;% at 0.4&#8201;% supersaturation, indicating hygroscopic nature of the dust. The vertical structure of CCN properties is found to be airmass-dependent; with higher activation efficiency even over the central IGP during the prevalence of marine airmass. Precipitation episodes seem to reduce the CCN activation efficiency below cloud level. An empirical relation has emerged between the CCN concentration and the scattering aerosol index (AI), which would facilitate prediction of CCN from aerosol optical properties.</p>