In the present study, total suspended particulate matter (TSP) samples were collected at 47 different sites (47 grids of 5 × 5 km2 area) of Delhi during winter (January-February 2019) in campaign mode. To understand the spatial variation of sources, TSP samples were analyzed for chemical compositions including carbonaceous species [organic carbon (OC), elemental carbon (EC) and water-soluble organic carbon (WSOC)], water-soluble total nitrogen (WSTN), water-soluble inorganic nitrogen (WSIN), polycyclic aromatic hydrocarbons (16 PAHs), water-soluble inorganic species (WSIS) (F−, Cl−, SO42−, NO2−, NO3−, PO43−, NH4+, Ca2+, Mg2+, Na+, and K+), and major & minor trace elements (B, Na, Mg, Al, P, S, Cl, K, Ca, Ti, Fe, Zn, Cr, Mn, Cu, As, Pd, F, and Ag). During the campaign, the maximum concentration of several components of TSP (996 µg/m3) was recorded at the Rana Pratap Bagh area representing a pollution hotspot of Delhi. The maximum concentrations of PAHs were recorded at Udhyog Nagar, a region close to heavily loaded diesel vehicles, small rubber factories, and waste burning areas. Higher content of Cl− and Cl−/Na+ ratio (> 1.7) suggests the presence of nonmarine anthropogenic sources of Cl− over Delhi. Minimum concentrations of OC, EC, WSOC, PAHs, and WSIS in TSP were observed at Kalkaji representing the least polluted area in Delhi. Enrichment factor < 5.0 at several locations and a significant correlation of Al with Mg, Fe, Ti, and Ca and C/N ratio indicated the abundance of mineral/crustal dust in TSP over Delhi. Principal component analysis (PCA) was also performed for the source apportionment of TSP and extracted soil dust was found to be the major contributor to TSP followed by biomass burning, open waste burning, secondary aerosol, and vehicular emissions.