Improving urban air quality is a global challenge. To implement successful abatement measures that reduce atmospheric particulate matter (APM) and associated metal concentrations, precise source apportionment is needed. For this, apportioning contributions from coal and biomass burning and differentiating these from non-exhaust traffic emissions in urban APM is critical. Recent studies characterising the metal isotope composition of urban APM, and potential source materials suggested that non-traditional isotope systems could prove unique fingerprinting tools. Zinc isotopes should be able to separate APM derived from uncontrolled combustion (fly ash, isotopically heavy) from non-exhaust traffic sources (tyre and brake wear, intermediate) and from controlled industrial emissions (flue gas, light). To test this hypothesis, we determined zinc isotope ratios of APM (TSP, PM2.5, PM1) in Beijing (coal combustion for residential heating) and Varanasi (biomass burning in pre-monsoon periods). In Beijing, δ66ZnLyon values of PM2.5 ranged from −0.41 to +1.01‰ in 2015 (avg = +0.25 ± 0.50‰, n = 19). Aerosols (including TSP, PM2.5 and PM1 samples) from the heating period were significantly (t-test, p < 0.001) heavier (avg = +0.90 ± 0.12‰, n = 7) than those from the non-heating period (avg = +0.14 ± 0.36‰, n = 23). Average δ66ZnLyon values of PM2.5 in Varanasi in spring 2015 were +0.82 ± 0.11‰ (n = 4). Extent and direction of isotope fractionation is in line with that expected from theoretical models and the isotope signatures observed agree with previously determined ratios of source materials. Our study links for the first time comprehensively the heavy zinc isotope compositions in APM to coal and biomass burning and shows that zinc isotope compositions of aerosols can discriminate between non-exhaust traffic and combustion sources.