Computer-controlled scanning electron microscopy (CCSEM) has been assessed for the determination of form and size distribution of heavy metals in urban contaminated soils. Metal distributions within individual particles were determined using X-ray element mapping. The sites selected for study were (1) around a landfill site, previously a colliery in Wolverhampton, UK and (2) a private garden adjacent to a railway in Nottingham, UK. Backscattered thresholding techniques were used to isolate the Pb-containing categories. The classification results for both Wolverhampton and Nottingham soils were generally similar but more Pb-containing classes were observed for the Nottingham samples when a comparison was made between results of the same size fractions. However, difficulties with the technique arose when particles showing chemically similar weathering crusts were assigned to the same class, despite having different internal compositions. The CCSEM data therefore need to be interpreted with caution and their application limited to situations in which particle internal complexity is not an issue.