Identifying the contamination and sources of potentially toxic elements (PTEs) in road-dust sediment (RDS) and the surrounding greenspace soil of urban environments and understanding their ecological-health risks are important for pollution management and public health. The contamination characteristics, ecological and probabilistic health risks, and source apportionment of eight PTEs (Cd, Pb, Cr, Cu, Ni, As, Zn, and Hg) in the Yellow River Custom Tourist Line of Lanzhou, which is the largest open urban riverfront scenic park in China, were investigated. The results showed that all the RDS PTE mean concentrations exceeded their soil background values, whereas for the surrounding greenspace soils, the concentrations of the PTEs, except for Cr and Ni, were also higher than their local background levels. Moreover, the RDS-soil system was mainly contaminated by Cd, Zn, Pb, Cu, and Hg to varying degrees, and the integrated ecological risks of PTEs in the RDS and soil were high and considerable at most sites, respectively. The probabilistic health risk assessment results demonstrated that the non-carcinogenic hazard risk for humans was negligible, but the total carcinogenic risks should be considered. Source apportionment using a positive matrix factorization model combined with multivariate statistical analyses revealed that Cr, Ni, and As in the RDS-soil system were from natural and industrial sources, Cd, Pb, Zn, Cu came from vehicle emissions and pesticide and fertilizer applications, and Hg was from natural and industrial sources and utilization of pesticides with fertilizers. This work provides scientific evidence for urban planning and human health protection in urban environments.