Water-soluble inorganic ions (WSII), organic carbon (OC) and elemental carbon (EC) and metals in residue of water-soluble fraction were studied in fine (PM2.5) and coarse (PM2.5-10) particles duirng winter season over two urban cities Amritsar (AMS) and New Delhi (DEL) in norh India. PM2.5/PM2.5-10 mass ratios at DEL and AMS were 3.6 and 2.79, respectively. ∑WSIIs was nearly 25% of total mass in two size fractions and were higher in PM2.5 compared to PM2.5-10 at both sites. Secondary ions SO42– and NH4+ were dominant at both sites. Adsorption of fine particles onto the larger particles could be possible source of soluble ions in PM2.5-10. SO42–, NO3– were neutralized by NH4+ and formation of (NH4)2SO4 dominated over NH4NO3 in PM2.5, and by Ca2+ in PM2.5-10 over DEL. Coal burning, and agriculture and livestock emissions were potential sources of precursor gases of SO42– and NH4+. Plastic burning and brick kiln industry contributed Cl– in PM2.5. OC dominated over EC over both sites and total carbon (OC + EC) was more over AMS compared to DEL. Low temperature burning dominated over high temperature as indicated by more Char-EC than soot-EC. OC, EC and K+ were contributed by biomass burning over AMS whereas they were sourced from multiple sources over DEL. The Al normalized ratio of elements in sample to crust were more in PM2.5 compared to PM2.5-10. Fe, Ti, Mn ratio of < 1 was attributed to silica dilution effect. Pb, Cu and Zn ratios in PM2.5 were 63, 18 and 13 over DEL and 2, 11 and 31 over AMS, respectively. Ba and Zn were contributed by vehicular emissions. The coefficient of divergence value of > 0.5 indicated the spatial heterogeneity in particle chemistry between two sites. Biomass burning and re-suspension of dust should be restricted to improve air quality and safeguard human health.