Concentrations of cadmium, chromium, copper, nickel, lead, and zinc in agricultural soils at 32 sites in the Lihe River Watershed of the Taihu region, East China, and their potential ecological risks and possible sources were investigated. Enrichment factor analysis demonstrated enrichment in the order Cd > Pb > Zn > Cu > Ni > Cr. The potential ecological risk index and risk assessment code analyses indicated that, of the metals studied, Cd posed the most significant ecological risk in the study area. Statistical analyses, GIS mapping, and enrichment factor analysis suggested that Cd, Pb, Cu, and Zn were derived mainly from anthropogenic sources, including agricultural, industrial, and vehicular emissions, while Cr and Ni were mainly from natural sources. Positive matrix factorization revealed that Cd, Cr, Cu, Ni, Pb, and Zn were sourced from industrial and vehicular emissions (73.7%, 21.3%, 71.4%, 20.3%, 75.0%, and 62.2%, respectively), the agricultural sector (26.3%, 36.3%, 6.8%, 38.9%, 15.7%, and 6.9%, respectively), and parent materials (0%, 42.4%, 21.8%, 40.8%, 9.2%, and 30.9%, respectively). It was recommended that strategies be implemented to reduce industrial point-source pollution.