Atmospheric Brown Clouds (ABC), regional‐scale haze events, are a significant concern for both human cardiopulmonary health and regional climate impacts. In order to effectively mitigate this pollution‐based phenomenon, it is imperative to understand the magnitude, scope and source of ABC in regions such as South Asia. Two sites in S. Asia were chosen for a 15‐month field campaign focused on isotope‐based source apportionment of carbonaceous aerosols in 2008–2009. Both the Maldives Climate Observatory in Hanimaadhoo (MCOH) and a mountaintop site in Sinhagad, India (SINH) act as regionally mixed receptor sites. Annual radiocarbon‐based source apportionment for soot elemental carbon (SEC) at MCOH and SINH revealed 73 ± 6% and 59 ± 5% contribution from biomass combustion, respectively (remainder from fossil fuel). The contributions from biogenic/biomass combustion to total organic carbon were similar between MCOH and SINH (69 ± 5% and 64 ± 5, respectively). The biomass combustion contribution for SEC in the current study, especially the results from MCOH, shows good agreement with published black carbon emissions inventories for India. Geographic source assessment, including clustered back trajectory analysis and carbon contribution by source region, indicated that the highest SEC/TOC loads originated from the W. Indian coastal margin, including the coastal city of Mumbai, India. The winter dry season ¹⁴C‐based source apportionment of the BC‐tracing SEC fraction for 2006, 2008, 2009 were not statistically different (p = 0.7) and point to a near‐constant two‐thirds contribution from biomass combustion practices, including wood and other biofuels as well as burning of agricultural crop residues.