High-altitude terrain may intersect the upper atmospheric boundary layer and exhibit distinct environmental dynamics. We investigated the anthropogenic pollutants polychlorinated alkanes (PCAs, also known as chlorinated paraffins) in surface soils along a transect from the La Paz-El Alto metropolitan area in Bolivia (3200–4100 masl) to the upper slopes of Mount Chacaltaya (>5200 masl), around 16 km away. Concentrations of PCAs in urban soils (750–5,230 ng/g organic carbon [OC]) decreased exponentially with increasing distance from the urban boundary, declining to ∼150 ng/g OC at elevations below 4,700 masl. Beyond 4,700 masl concentrations increased again, reaching levels comparable to those in the urban area, 1,670–4,300 ng/g OC, above 5,000 masl. Given that pollutant concentrations typically decline with distance from their source, this altitudinal trend, together with a pronounced shift in PCA forensic fingerprints near 4,700 masl, strongly suggests contributions from sources beyond the local metropolitan area. Carbon and nitrogen isotope signatures in organic carbon further support long-range transport as a source, consistent with previous modeling and observations that the upper slopes of Mount Chacaltaya predominantly receive air masses and organic carbon from distant regions via transport in the free troposphere. Our observation that pollutant levels in high-altitude areas are comparable to those in the metropolis of 1.8-million inhabitants underscores the efficiency of long-range atmospheric transport.