This study reports spatial and temporal variability of Zn and Cu isotopes in atmospheric particulate matter (PM) collected in two major European cities with contrasting atmospheric pollution, Barcelona and London. We demonstrate that non-traditional stable isotopes identify source contributions of Zn and Cu and can play a major role in future air quality studies. In Barcelona, fine PM were collected at street level at sites with variable traffic density. The isotopic signatures ranged between −0.13±0.09 and −0.55±0.09‰ for d66ZnIRMM and between +0.04±0.20 and +0.33±0.15‰ for d65CuAE633. Copper isotope signatures similar to Cu sulphides and Cu/Sb ratios within the range typically found in brake wear suggest that non-exhaust emissions from vehicles are dominant. Negative Zn isotopic signatures characteristic for gaseous emissions from smelting and combustion and large enrichments of Zn and Cd suggest contribution from metallurgical industries. In London, coarse PM collected on the top of a building over 18 months display isotope signatures ranging between +0.03±0.04 and +0.49±0.02‰ for d66ZnIRMM and between +0.37±0.17 and +0.97±0.21‰ for d65CuAE633. Heavy Cu isotope signatures (up to +0.97±0.21‰) and higher enrichments and Cu/Sb ratios during winter time suggest important contribution from fossil fuel combustion. The positive d66ZnIRMM signatures are in good agreement with signatures characteristic for ore concentrates used for the production of tires and galvanised materials, suggesting non-exhaust emissions from vehicles as the main source of Zn.