This study aims to increase our current knowledge on the concentration of particulate-bound mercury (PBM) in urban environments of three Iranian cities, where high concentrations of dust particles can act as carriers for mercury transport and deposition. A total of 172 dust samples were collected from Ahvaz, Asaluyeh, and Zabol residential houses and in outdoor air and were analyzed for total mercury content. Ahvaz is a highly industrialized city with large metallurgical plants, refineries, and major oil-related activities, which were assumed to contribute to elevated contents of PBM in this city. Very high levels of Hg contamination in Ahvaz indoor dust samples were calculated (Contamination Factor: CF > 6). Sampling sites in Asaluyeh are influenced by Hg emissions from the South Pars Gas Field. However, the results revealed a relatively lower concentration of PBM in Asaluyeh, with a low-to-moderate level of Hg contamination. This is likely ascribed to the lower content of total mercury in hydrocarbon gases than crude oil, in addition to the absence of metal smelting plants in this city compared to Ahvaz. Zabol, as a city devoid of industrial activity, presented the lowest levels of PBM concentration and contamination. Indoor dust in Ahvaz showed considerable potential to cause a non-carcinogenic health risk for children, mainly through the inhalation of PBM, while the health risk for other cities was below safe limits. The trend of health risk was found in the order of indoor > outdoor and children > adults in all studied cities.