Abstract. Volatile organic compounds (VOCs) and particulate matter (PM) are major constituents of smog. Delhi experiences severe smog during the post-monsoon season, but a quantitative understanding of VOCs and PM sources is still lacking. Here, we conduct a source apportionment study for VOCs and PM using a recent (2022), high-quality dataset of 111 VOCs, PM2.5, and PM10 in a positive matrix factorization (PMF) model. Contrasts between clean monsoon air and polluted post-monsoon air, VOC source fingerprints, and molecular tracers enabled us to differentiate paddy residue burning from other biomass-burning sources, which had previously been impossible. Burning of fresh paddy residue, as well as residential heating and waste burning, contributed the most to observed PM10 levels (25 % and 23 %, respectively) and PM2.5 levels (23 % and 24 %, respectively), followed by heavy-duty vehicles fuelled by compressed natural gas (CNG), with a PM10 contribution of 15 % and a PM2.5 contribution of 11 %. For ambient VOCs, ozone formation potential, and secondary-organic-aerosol (SOA) formation potential, the top sources were petrol four-wheelers (20 %, 25 %, and 30 %, respectively), petrol two-wheelers (14 %, 12 %, and 20 %, respectively), industrial emissions (12 %, 14 %, and 15 %, respectively), solid-fuel-based cooking (10 %, 10 %, and 8 %, respectively), and road construction (8 %, 6 %, and 9 %, respectively). Emission inventories tended to overestimate residential biofuel emissions at least by a factor of 2 relative to the PMF output. The major source of PM pollution was regional biomass burning, while traffic and industries governed VOC emissions and secondary-pollutant formation. Our novel source apportionment method even quantitatively resolved similar biomass and fossil fuel sources, offering insights into both VOC and PM sources affecting extreme pollution events. This approach represents a notable advancement compared to current source apportionment approaches, and it could be of great relevance for future studies in other polluted cities and regions of the world with complex source mixtures.