This study reports for the first time a comprehensive analysis of nitrogenous and carbonaceous aerosols in simultaneously collected PM2.5 and TSP during pre-monsoon (March–May 2018) from a highly polluted urban Kathmandu Valley (KV) of the Himalayan foothills. The mean mass concentration of PM2.5 (129.8 µg/m3) was only ~25% of TSP mass (558.7 µg/ m3) indicating the dominance of coarser mode aerosols. However, the mean concentration as well as fractional contributions of water-soluble total nitrogen (WSTN) and carbonaceous species reveal their predominance in find-mode aerosols. The mean mass concentration of WSTN was 17.43±4.70 µg/m3 (14%) in PM2.5 and 24.64±8.07 µg/m3 (5%) in TSP. Moreover, the fractional contribution of total carbonaceous aerosols (TCA) is much higher in PM2.5 (~34%) than that in TSP (~20%). The relatively low OC/EC ratio in PM2.5 (3.03 ± 1.47) and TSP (4.64 ± 1.73) suggests fossil fuel combustion as the major sources of carbonaceous aerosols with contributions from secondary organic aerosols. Five-day air mass back trajectories simulated with the HYSPLIT model, together with MODIS fire counts indicate the influence of local emissions as well as transported pollutants from the Indo-Gangetic Plain region to the south of the Himalayan foothills. Principal component analysis (PCA) also suggests a mixed contribution from other local anthropogenic, biomass burning, and crustal sources. Our results highlight that it is necessary to control local emissions as well as regional transport while designing mitigation measures to reduce the KV’s air pollution.