The concentrations of particulate matter and Fe in airborne particulate matter and transplanted moss were investigated to evaluate the air quality of Tirana city. It was carried out in the summer of 2021 and the winter of 2020-2021. Particulate matter of various sizes (PM2.5 and PM10) was collected on Teflon-coated glass fibre filters. Fe was determined in PMs and moss transplants, the last were exposed for two months at the same monitoring site as PMs. The measurements were carried out in areas with heavy traffic during the summer under relatively high air temperatures, up to 23° C, which can affect the high concentrations of solid particles in the air and therefore high Fe levels. Statistical analysis was used to discuss the results of particulate matter and iron in solid particles and moss. A higher concentration of Fe was found in total suspended particles (TSP) and a lower concentration in smaller particles. The concentration data were compared with the recommended values in the European Directives. The concentrations of all parameters under investigation were higher than the permitted ones for rural and residential areas and lower than the recommended values for industrial areas. Correlation analysis revealed high and significant correlations (R > 0.8, p < 0.05) between Fe concentrations in moss transplants and particulate matter, showing a high effect of particulate matter on airborne Fe. It may increase human exposure through inhalation and lead to harmful health problems. This requires stronger measures to improve air quality in the city.