Characteristics and sources of volatile organic compounds (VOCs) were investigated with highly time-resolved simultaneous measurements by two proton-transfer-reaction time-of-flight mass spectrometers (PTR-ToF-MS) at an urban and a suburban site in New Delhi, India, from January to March 2018. During the measurement period, high mixing ratios of VOCs and trace gases were observed, with high nocturnal mixing ratios and strong day-night variations. The positive matrix factorization (PMF) receptor model was applied separately to the two sites, and six major factors of VOCs were identified at both sites, i.e., two factors related to traffic emissions, two to solid fuel combustion, and two secondary factors. At the urban site, traffic-related emissions comprising mostly mono-aromatic compounds were the dominant sources, contributing 56.6% of the total mixing ratio, compared to 36.0% at the suburban site. Emissions from various solid fuel combustion processes, particularly in the night, were identified as a significant source of aromatics, phenols and furans at both sites. The secondary factors accounted for 15.9% of the total VOC concentration at the urban site and for 33.6% at the suburban site. They were dominated by oxygenated VOCs and exhibited substantially higher contributions during daytime.