A test site located along a 12-lane motorway east of Montpellier, France, is used to evaluate the potential of biomagnetic monitoring on traffic-related particulate matter (PM) to parametrize a computational fluid dynamics (CFD) simulation of the local airflow. Two configurations were established on the site with three vegetated flat-top earth berms of a basic design, and a fourth one was located windward to the traffic roofed with a 4-m-high precast concrete wall. As a first step, PM deposition simultaneously on plant leaves, on low-cost passive artificial filters, and on soils was estimated from proxies supplied by magnetic and X-ray fluorescence measurements on both sides of the motorway. These latter revealed that traffic-related pollutants are present on soils samples highlighted with a clear fingerprint of combustion residues, and wears of breaks, vehicles, and highway equipment. Maximum PM accumulations were detected in the lee of the berm–wall combination, while no significant deposition was observed on both sides of the flat-top earth berms. These results are in line with measurements from PM µ-sensors operated by the regional state-approved air quality agency. Finally, we compared the experimental measurements with the outcomes of a computational fluid dynamics (CFD) modeling based on the Reynolds-Averaged Navier–Stokes (RANS) equations that consider the traffic-induced momentum and turbulence. The CFD modeling matches the experimental results by predicting a recirculated flow in the near wake of the berm–wall combination that enhances the PM concentration, whereas the flat-top berm geometry does not alter the pollutants’ transport and indeed contributes to their atmospheric dispersion.