Atmospherically derived organic films have been found on an impervious surface along an urban-rural gradient in the Toronto, Ontario, Canada area. Film thickness and concentrations, expressed on an aerial basis, of sigman-alkanes, sigmaPCB, sigmaPAH, and sigmaOC (organochlorine) pesticides decrease along this gradient, coincident with lower atmospheric emissions (PCB and PAH) and less accumulation in thinner rural films (OC pesticides). For PCBs and some OC pesticides, patterns of chemical abundance also shift, indicating a "fresh" pattern near emission sources (downtown) versus aged patterns at rural locations that are indicative of atmospheric transport. Plant-derived n-alkane concentrations were greater at urban than rural sites, and we hypothesize greater urban plant wax production and erosion due to air pollution. As expected, along the urban-rural gradient the concentration of particle-phase PAH decreased more rapidly than that of gas-phase compounds, but unexpectedly the contribution of alkylated PAH increased from urban to rural locations. Distances over which concentrations decline by 63% vary from 50 km for persistent gas-phase compounds (e.g., P1,2CB) to 10-20 km for reactive gas-phase compounds (e.g., naphthalene, fluoranthene) to <5-10 km for particle-phase compounds (e.g., P6-10CB, benzo[b]fluoranthene, benzo[e]pyrene).