Urbanization significantly influences soil and environmental quality through increased anthropogenic activities. In our study we evaluated soil metal pollution along an urbanization gradient in Vienna by analyzing topsoil samples from urban, suburban, and rural areas using ICP-OES. Increased concentrations of Cu, Pb, Sr, and Zn were observed in urban and suburban soils, indicating anthropogenic inputs primarily associated with traffic emissions. Pollution index (PI) assessment revealed moderate contamination by Cd (1 ≤ PI ≤ 2) and low pollution levels for Cr, Cu, Ni, Pb, and Zn (PI ≤ 1). Additionally, tree species were examined for air pollution sensitivity using the Air Pollution Tolerance Index (APTI) and leaf heavy metal concentrations. Based on APTI values, the studied species were sensitive indicators of air pollution; thus, they are useful bioindicator species, and they are suitable for air pollution monitoring. Comparative observations from Faisalabad showed similarly increased metal concentrations in urban soils, the bioaccumulation factor (BAF) was used to assess metal accumulation in the soil and leaves of the neem tree (Azadirachta indica) in Faisalabad, Pakistan. Our findings show that high concentrations in soil do not always turn into higher plant uptake for plants. Our results suggest that traffic and industrial emissions are likely the main cause of the metals in Faisalabad, because their concentration is higher than their background concentration. Overall, the findings emphasize the effectiveness of soil and plant elemental analyses, along with pollution indices, as reliable tools for assessing environmental contamination in urban ecosystems.