The current work aimed to discriminate urban pollution sources using the zinc isotope ratio as a tracer. The study was conducted on the example of the large industrial city of Ekaterinburg, Russia. The urban surface-deposited sediment (USDS) collected in the multistory residential areas was analyzed as a geoindicator. The USDS represents a geochemical trap in an urban environment and reflects an area’s contemporary urban geochemical conditions and their changes over time. USDS samples were collected from an irregular grid in the city during 2007–2010. Sample decomposition was conducted using a mixture of acids (HF, HNO3, and HCl). Zn isotope ratios were measured using MC-ICP-MS Neptune Plus (Thermo Fischer, Germany). The isotope ratios were reported as δ66Zn relative to the JMC-Lyon certified isotopic standard. Zinc isotope ratios in USDS samples varied from −1.00 to +0.49‰. 84% of investigated USDS samples in Ekaterinburg have a zinc isotope ratio, corresponding to road traffic and non-exhaust emissions (−0.50 to +0.49‰). The δ66Zn values in the residential districts near the city's railway were −1.0 to −0.6‰; the value near the Railway Station was −0.29‰; next to highways were from −0.5 to −0.3‰.