The ecological risk assessment and source identification of heavy metals (HMs) are significant for resource utilization and food security. This study aims to assess the spatial distributions, potential sources, and ecological risks of HMs in stream sediments in Zambia. Using 735 samples collected from stream sediments across the country and methods such as inductively coupled plasma mass spectrometry (ICP-MS), atomic fluorescence spectrometry (AFS), and X-ray fluorescence spectrometry (XRFS), this study determined the concentrations of the seven HMs, i.e., arsenic (As), chromium (Cr), copper (Cu), mercury (Hg), nickel (Ni), lead (Pb), and zinc (Zn). The spatial distributions of these HMs were determined using a Geographic Information System (GIS), and their ecological risks were accessed based on the analytical results of their potential sources. Additionally, this study explored the relationships between mining activities and regions with high heavy metal (HM) concentrations based on the statistical analysis of the HM concentrations and geology of the study area. The results indicate the stream sediments in Zambia exhibit average As, Cr, Cu, Hg, Ni, Pb, and Zn concentrations of 1.49 × 10−6, 19.34 × 10−6, 12.12 × 10−6, 12.70 × 10−9, 7.13 × 10−6, 12.52 × 10−6, and 16.30 × 10−6, respectively. The analytical results of the geoaccumulation index (Igeo) and potential ecological risk index (PERI) reveal the presence of relatively high As and Cu concentrations, especially in Copperbelt and North-Western provinces and areas surrounding Lusaka—the capital of Zambia. The HM contamination in stream sediments in Zambia is primarily caused by Cu and gold (Au) mining. This study exemplifies how to determine potential sources and ecological risks of HMs in stream sediments, holding important implications for nation-scale environmental contamination prevention and land utilization planning.
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