The hazardous element (HE) pollution of urban surface dust is a serious environmental issue, due to its toxicity and potential hazardous effects. Surface dust samples were collected from core urban, urban, and suburban gradients in the city of Urumqi in arid northwestern China, and the concentrations of six HEs, such as arsenic (As), cadmium (Cd), nickel (Ni), lead (Pb), mercury (Hg), and chromium (Cr) were determined. The pollution load index (PLI) and the US EPA health risk assessment model were applied, to assess and compare the pollution levels and the potential health risk of HEs in the surface dust in different urbanization gradients. The results indicated that the average concentrations of Hg, Cd, and Ni in the surface dust decreased in the order of core urban > urban > suburban, whereas the average concentrations of As, Cr, and Pb decreased in the order of urban > core urban > suburban. The PLI of HEs in surface dust decreased in the order of core urban > urban > suburban. The concentrations of HEs in the core urban and urban gradients were relatively higher than those in the suburban gradient. Furthermore, the total non-carcinogenic and carcinogenic risk index of the investigated HEs in surface dust decreased in the order of urban > core urban > suburban, for both adults and children. In addition, the pollution of surface dust by HEs in all urbanization gradients was more harmful to children’s health than to adults’. Overall, the potential non-carcinogenic and carcinogenic health risk of the investigated HEs, instigated primarily via the oral ingestion of surface dust, was found to be within the acceptable range. However, urbanization has effected the accumulation of HEs in surface dust, and Cr was the main non-carcinogenic risk factor, whereas Cd was the main carcinogenic risk factor, among the analyzed HEs in surface dust in three urban gradients in the study area.