Toxic trace element (TTE) contamination in urban soils may pose potential health risks, especially in cities with previous industrial activities. This study aimed to investigate soil contamination in urban allotments in Sheffield, the uptake of TTEs in autumn and spring sown onions (Allium cepa), and their potential risks on human health via consumption of the crops. Paired soil and plant samples were taken in triplicates from four private allotments to assess potentially elevated levels of lead (Pb), zinc (Zn), copper (Cu), arsenic (As), and chromium (Cr). These elements in soils exceeded the ambient background levels for England. Both Pb and As exceeded some UK and EU soil tolerable limits. Concentration factors (CF) were calculated as the ratio of trace element in the plant as compared to that in the soil, and uptake rates were in the order Zn>Cu>Cr>Pb>As. Concentrations were higher for most TTEs in spring sown onions (SSO), and had significantly higher CF (p < 0.05) for Pb and Cr than autumn sown onions (ASO), whereas the opposite was true for As. Toxic elements in plants did not exceed FAO/WHO intake limits when considering TTE content per plant and consumption rates. Human health risk assessment calculations using target hazard quotients (THQ) and hazard indexes (HI) indicated that consuming onions alone did not pose an immediate health risk.