This study identifies factors influencing spatial and temporal variations in magnetic susceptibility and heavy metal content in soils and airborne particulate matter within the Kyiv megapolis, Ukraine, and highlights how source apportionment differs in the long and short run. Topsoil magnetic susceptibility anomalies of > 70 × 10−8 m3kg−1 are observed around old factories. The tree bark magnetic susceptibility map provides a record of industry general low emissions for the last 2–3 decades. The patterns of both spatial distributions confirm that factory emissions dominate the composition of particulate falling on the ground in urban area, with exclusion of streets with heavy traffic. Enhanced concentrations of Cu, Ni, and Zn have been found in urban soils, showing a positive correlation with magnetic susceptibility. Re-suspended road dust dominates temporal variation of particulate matter magnetic susceptibility collected on air filters. The air at busy streets is cleaner in winter, when the street dust gets immobilized by snow cover or freezing. Industries in Kyiv pose no significant effect on air quality; the concentrations of Cr, Ni, Cu, Zn, Cd, and Pb are at normal urban level with the exception of the near vicinity to factories. Air in streets with heavy traffic is enriched with Fe and Mn. Principal component analysis reveals different pattern of air pollution for the busy streets and yard areas. Yards are less affected by road dust; thus, contribution of industrial emissions can be distinguished. The results provide context for further quantification of any alterations in ecological state of Kyiv megapolis that may have arisen from socio-economic shocks and direct threats connected to the current war.