Airborne particulate matter is a serious threat to human health, especially in fast-growing cities. In this study, we carried out a magnetic and elemental study on tree leaves used as passive captors and urban dust from various sites in the city of Santiago, Chile, to assess the reliability of magnetic and elemental measurements to characterize particulate matter pollution from vehicular origin. We found that the magnetic susceptibility and saturation isothermal remanent magnetization measured on urban tree leaves is a good proxy for tracing anthropogenic metallic particles and allow controlling the exposure time for particulate matter collection, in agreement with other studies carried out in large cities. Similar measurements on urban soil can be influenced by particles of detritic (natural) origin, and therefore, magnetic measurements on tree leaves can help to identify hotspots where fine particles are more abundant. Elemental particle-induced X-ray emission analysis of tree leaves showed the presence of a number of elements associated with vehicular emissions, in particular Cu, Zn, Fe, K and S which are present at every site, and As, Se, V, Ni, Sr, Zr, Mo and Pb identified at some sites. We observed a correlation between magnetic parameters and the concentrations of S and Br as well as Cu to a smaller extent. Moreover, this study shows the importance of selecting carefully the tree species as well as the location of trees in order to optimize phytoremediation.