Delhi is one among the highly air polluted cities in the world. Absence of causal relationship between emitting sources of PM and their impact has resulted in inadequate actions. This research combines a set of innovative and state-of-the-art analytical techniques to establish relative predominance of PM sources. Air quality sampling at six sites in summer and winter for 40 days (at each site) showed alarmingly high PM concentrations (340 ± 135 μg/m). The collected PM was subjected to chemical speciation including ions, metals, organic and elemental carbons which followed application of chemical mass balance technique for source apportionment. The source apportionment results showed that secondary aerosols, biomass burning (BMB), vehicles, fugitive dust, coal and fly ash, and municipal solid waste burning were the important sources. It was observed that secondary aerosol and crustal matter accounted for over 50% of mass. The PM levels were not solely result of emissions from Delhi; it is a larger regional problem caused by contiguous urban agglomerations. It was argued that emission reduction of precursors of secondary aerosol, SO, NO, and volatile organic compounds, which are unabated, is essential. A substantial reduction in BMB and suspension of crustal dust is equally important to ensure compliance with air quality standards.