Lahore, Pakistan is an emerging megacity that is heavily polluted with high levels of particle air pollution. In this study, respirable particulate matter (PM2.5 and PM10) were collected every sixth day in Lahore from 12 January 2007 to 19 January 2008. Ambient aerosol was characterized using well-established chemical methods for mass, organic carbon (OC), elemental carbon (EC), ionic species (sulfate, nitrate, chloride, ammonium, sodium, calcium, and potassium), and organic species. The annual average concentration (+/- one standard deviation) Of PM2.5 was 194 +/- 94 mu g m(-3) and PM10 was 336 +/- 135 mu g m(-3). Coarse aerosol (PM10-2.5) was dominated by crustal sources like dust (74 +/- 16%, annual average +/- one standard deviation), whereas fine particles were dominated by carbonaceous aerosol (organic matter and elemental carbon, 61 +/- 17%). Organic tracer species were used to identify sources Of PM2.5 OC and chemical mass balance (CMB) modeling was used to estimate relative source contributions. On an annual basis, non-catalyzed motor vehicles accounted for more than half of primary OC (53 +/- 19%). Lesser sources included biomass burning (10 5%) and the combined source of diesel engines and residual fuel oil combustion (6 +/- 2%). Secondary organic aerosol (SOA) was an important contributor to ambient OC, particularly during the winter when secondary processing of aerosol species during fog episodes was expected. Coal combustion alone contributed a small percentage of organic aerosol (1.9 +/- 0.3%), but showed strong linear correlation with unidentified sources of OC that contributed more significantly (27 +/- 16%). Brick kilns, where coal and other low quality fuels are burned together, are suggested as the most probable origins of unapportioned OC. The chemical profiling of emissions from brick kilns and other sources unique to Lahore would contribute to a better understanding of OC sources in this megacity. (C) 2009 Elsevier Ltd. All rights reserved.