A first-of-its-kind source apportionment study of the Ahmedabad, India aerosol was conducted in order to determine the major sources contributing to the measured total suspended particles (TSPs). TSP samples were collected approximately once every ten days between May 2000 and January 2003, and analyzed for TSP mass, anions, cations, and elemental concentrations. An advanced factor analysis technique, positive matrix factorization (PMF) was applied to the measured concentrations and six factors were resolved. The model resolved factors included airborne regional dust, calcium carbonate rich dust, biomass burning/vehicular emissions, secondary nitrate/sulfate, marine aerosol, and smelter. Among the resolved factors, airborne regional dust was the highest contributor to the measured TSP mass followed by calcium carbonate rich dust with their average contributions accounting for 57.9 and 19.0%, respectively. Thus, crustal factors were the most dominant sources of TSP in Ahmedabad accounting for nearly 77% of the mass. Potential source contribution function (PSCF) analysis identified parts of Madhya Pradesh and Uttar Pradesh, regions in southwestern Pakistan along the Indo-Gangetic Plain (IGP), and southern Iran as potential source locations for the airborne regional dust factor. In contrast, Rajasthan and Madhya Pradesh, and parts of northern Pakistan were identified as potential source locations for the calcium carbonate rich dust factor. It is hypothesized that aerosol contributions from several limestone quarries in Rajasthan and Madhya Pradesh may have resulted in this factor being calcium carbonate enriched.