Understanding the level of heavy metal contamination coupled with the assessment of environmental and human risks associated with mine waste dumpsites is an important step to initiating efficient measures for mine wasteland restoration, stabilization, and bioremediation. In the present study, concentration of the heavy metals; Copper (Cu), Cobalt (Co), Iron (Fe), Lead (Pb), Manganese (Mn), and Zinc (Zn) in soil from mine waste dumpsites around Kitwe (Sites: TD25 and TD26) and Mufulira (Site: TD10), Zambia, was assessed to determine the level of contamination, ecological risks, and progress made in reclamation. The mine waste dumpsites in the two towns are located in the vicinity of residential areas. Therefore, there is need to provide information for optimization of protocols for post-mining landscape in Zambia and elsewhere to limit soil, river, and groundwater contamination and to accelerate the restoration process . Mean values for soil pH, electrical conductivity, and organic matter varied between 5.9–8.4, 2534.8–538.6 μS/cm, and 0.90–2.75%, respectively. The mean concentrations of heavy metals of TD25, TD26, and TD10 decreased in order of Fe > Cu > Co > Mn > Pb > Zn across all sites. However, the order of overall degree of heavy metal contamination computed using control soil as a baseline in TD25, TD26, and TD10 was Cu > Co > Fe > Pb > Mn > Zn. The pollution load index was 0.355 at TD25, 0.329 at TD26, and 0.189 at TD10, indicating high soil pollution at TD25 and TD26. The Potential Ecological Risk Index for all heavy metals tested at TD25, TD26, and TD10 showed low ecological risk in the vicinity of the studied dumpsites. Furthermore, the present study also showed that the polluted soils around smelter sites and mine waste dumpsites are susceptible to dispersion by wind and water. Additionally, results from TD10 revealed that the initiated remediation of the tailings dam was somewhat successful. Finally, this study provided an updated status regarding the accumulation of heavy metals in mine waste dumpsites of Kitwe and Mufulira, Zambia and baseline information necessary to enhance post-mining landscape reclamation.