The presence of urban surface pollutants washed off by stormwater is a growing concern due to their adverse effects on receiving water quality. The stormwater quality mitigation strategies, therefore, should be based on the knowledge of the distribution and source apportionment of pollutants on urban surfaces. This study showcases the distribution of particulate-associated PAHs as a function of surface characteristic. Samples were obtained from six sites in the city of Dresden, Germany, using a wet vacuum sample-taking method. Both surface load (mg/m²) and solid-phase concentration (mg/g) of PAHs were determined. Results show that the highest surface load of ∑₁₆PAHs was found at a natural stone-paved pedestrian path with 34.5 μg/m². By contrast, the highest solid-phase concentration occurred at a high traffic load road with 36 mg/kg. Through a combined qualitative diagnostic ratio and quantitative principal component analysis with stepwise multiple linear regression (PCA-MLR) source apportionment, two significant contributors to PAH at vehicular roads were primarily identified as pyrogenic and petrogenic sources; 81.6% of the PAH burden was ascribed to pyrogenic sources including vehicle emission, coal, and wood combustions; 18.4% was attributed to petrogenic sources, such as spilled engine oil and vehicular tire debris. To minimize the adverse influence of surface sediments adsorbed PAHs to the receiving waters via stormwater runoff, a surface pavement-based city street sweeping strategy could be planned and optimized to remove hazardous materials from the impervious urban surfaces.