The adverse health effects resulting from exposure to contaminated soil on internally displaced populations in Mitrovica, Kosovo can be determined by how the potentially harmful elements are bound in the soils. Certainly this was the case for Pb, present at concentrations ranging from 624 to 46,900 mg/kg, and at bioaccessibilities ranging <5% to nearly 90%. To assess why the soil Pb might differ so markedly in terms of its bioaccessibility, computer controlled scanning electron microscopy (CCSEM) was employed to determine how the Pb was associated with other elements at the individual particle (IP) level in soils from the area. It was found that the Pb-bearing particle types were, for the most part, different in each sample. We consider these differences as the main control on Pb bioaccessibility in these soils. Pb solubility at the IP level was evaluated by examining Pb-particles from these soils in the electron microscope before and after successive immersions in a simulated gastric fluid. This analysis (differential IP analysis) confirmed the CCSEM characterization that Pb associated with other higher atomic number elements (Fe, Zn, Cu and Ni) was less soluble than when it was present as isolated phases (e.g., as carbonate) or when it was bound with lower atomic number elements (Na, Al, Si, K, Ca). The heterogeneity in solubility and composition of the Pb-particles suggested that the Pb originated from a range of different anthropogenic activities. The nature of these different anthropogenic activities created the wide differences in Pb-bioaccessibilty by producing Pb bound in many different forms in the soil particles. This type of Pb-particle characterization highlights the role CCSEM analysis, and IP acid extraction, can play in providing supporting evidence alongside bioaccessibility data for applications in human health risk assessment and management of contaminated soil.