Multi-elemental profiles in bark of green ash trees collected in three representative areas of Buenos Aires, Argentina and Montevideo, Uruguay, were assessed as potential air pollution indicators. Ten elements: Al, Ba, Cr, Cu, Fe, Mg, Mn, Ni, Pb, and Zn, were measured using inductively coupled plasma optical emissions spectrometry from 70 samples collected in different environments: central, residential and rural (reference site), in order to compare spatial patterns of metal concentration. The samples used as a control were collected from a nature reserve situated far away from any significant influences, not even a nearby road. The reference site (RF) exhibited the lowest concentrations of Al, Cr, Fe, Ni, Pb, and Zn. However, Ba and Mn showed similar concentrations in all measured sites. Magnesium is the only element that had a greater concentration in RF than at the other sites. Copper did not show any clear pattern. The Centre of Montevideo (MVD) showed higher concentrations of Al, Ba, Cr, Fe, Pb and Zn than the Centre of Buenos Aires (BA). In the A sectors, Montevideo (SAMVD) showed higher concentrations of Al, Cu, Mg, Ni, and Zn and lower concentrations of Ba, Cr, Fe, Mn, and Pb than Buenos Aires (SABA). In the B sectors, Montevideo (SBMVD) showed higher concentrations of Al, Ba, Cu, Fe, Pb, and Zn and lower concentrations of Cr and Mg than Buenos Aires (SBBA), but similar concentrations of Mn and Ni. The use of bark for biomonitoring metals allowed us to detect concentration differences related to the urban fabric and the different kinds of vehicles and their fuels. In the cities, the differences in metal concentrations detected in bark were more striking between the sectors than between centers, despite CBA being much larger than CMVD in population, extension and vehicular traffic.