The aim of this study was to evaluate the use of tree barks as a bioindicator of atmospheric pollution in areas of contrasting population densities and to associate the levels of elements found in this bioindicator with those obtained in fingernail samples collected from students living in the same study areas. Tree bark samples were collected from urban areas near highways in regions with high (Area A), intermediate (Area B), and low (Area C) population densities of Porto Alegre, Brazil, and evaluated for chemical elements concentration. Since these areas also differed in traffic density, NO2 was measured by passive sampling. For a comparative purpose, the elements were also determined in fingernail samples collected from students living in the same areas. Accumulated elements were determined by inductively coupled plasma mass spectrometry (ICP-MS) and principal component analysis (PCA) was used as a tool in exploratory data analysis to identify possible sources. We found that Ba, Cd, Co, Cu, Mg, Mn, Ni, Pb, Sb, Sr, V, and Zn were at higher concentrations in tree barks in Area A, while Cd, Co, Cu, Mg, Mn, Ni, and Sr were at higher levels in students' fingernails of Area A as well. Furthermore, concentrations of elements found in barks were associated with those identified in fingernails collected from students living in the same areas. PCA demonstrated that vehicular traffic explained 66.4% of the variance in tree bark and 50.8% of the variance in fingernails. NO2 levels were significantly different among the areas, what is consistent with their respective vehicular flow and population density. In conclusion, we found conformance of elements levels accumulated in barks and fingernails at three monitoring areas with different profiles. The amount of traffic-related elements accumulated appears to be associated with the degree of urbanization and vehicular flow. Overall, data suggests a relationship between fingernails and tree bark as bioindicators of exposure to metals from air pollution.