An investigation is reported of the degree of metal pollution in the sediments of Kafrain Dam and the origin of these metals. Fourteen sampling sites located at Kafrain Dam were chosen for collecting the surface, cutbank, and dam bank sediment samples. The sediment samples have been subjected to a total digestion technique and analyzed by atomic absorption spectrometer for metals including Pb, Zn, Cd, Ni, Co, Cr, Cu, Mn, and Fe. XRD analyses indicate that the sediments of Kafrain Dam are mainly composed of calcite, dolomite, quartz, orthoclase, microcline, kaolinite, and illite reflecting the geology of the study area. The enrichment factor (EF) and geoaccumulation index (I(geo)) have been calculated and the relative contamination levels assessed in the study area. The calculations of I(geo) are found to be more reliable than of those of EF. The enrichment of metals in the study area has been observed to be relatively high. I(geo) results reveal that the study area is not contaminated with respect to Ni, Co, Cr, Cu, and Mn; moderately to strongly contaminated with Pb; and strongly to extremely contaminated with Cd and Zn. The high contents of Pb, Cd, and Zn in the study area result from anthropogenic activities in the catchment area of the dam site. These sources mainly include the agricultural activities, sewage discharging from various sources within the study area (effluent of wastewater treatment plants, treated and untreated wastewaters, and irrigation return water), and the several industries located in the area. Degrees of correlations among the various metals in the study area are suggested by the results and the intermetallic relationship.