In this study, the concentrations of Zn, Cr, Ni, Cu, Pb, As, Cd, and Hg in the surface sediments of 94 sites sampled from six water systems in the Lake Taihu Basin in China were measured, and the pollution risks and sources of the metals were identified. The results showed that the mean concentrations of Zn, Cr, Ni, Cu, Pb, As, Cd, and Hg in the riverine surface sediments were 163.6, 102.5, 45.5, 44.7, 37.0, 13.3, 0.5, and 0.1 mg/kg, respectively, higher than the corresponding background values (except for Hg). According to the geoaccumulation index (I), the Pb, Ni, Zn, Cu, and Cd concentrations in the riverine surface sediments were generally at low levels of pollution. Based on a pollution load index (PLI) evaluation, the Pb, Ni, Zn, and Cu concentrations in the riverine surface sediments were generally at moderate levels of pollution. According to the thresholds of potential ecological risk, the Cd and Hg concentrations in the riverine surface sediments exhibited moderate potential ecological risks. Multivariate statistical analysis indicated that the Pb in the riverine surface sediments primarily originated from domestic sewage, agricultural wastewater discharge, and petroleum combustion; the concentrations of Cr, Ni, and Zn were influenced by the electroplating and alloy manufacturing industries; the concentrations of Cu and As mainly originated from pesticide use and industrial wastewater discharge; and those of Cd and Hg primarily stemmed from industrial wastewater discharge. This research provides information regarding metallic contamination and the possible associated ecological risks to benthic organisms in the surface sediments of river systems and is useful for developing sustainable strategies for environmental pollution control and management in the Lake Taihu Basin.