The large-sized Tarangaole uranium deposit and its neighboring Daying and Nalinggou deposits, located in the northeastern margin of the Ordos Basin, constitutes a major uranium resource base in northern China. In order to further clarify the sedimentary material source, uranium source and regional sediment-tectonic setting of the uranium-fed clastic rocks (i.e., Zhiluo Formation(J(2)z)) in the district, this paper carried out whole-rock geochemistry, heavy minerals composition and in situ U-Pb dating of detrital zircons for sandstones from the lower section of the Zhiluo Formation. The results have shown that the average chemical differentiation index (CIA) for the host rocks is 73.16 and the chemical weathering degree is moderate. Heavy minerals are mainly composed of ilmenite, garnet, chlorpyrite, zircon, pyrite, apatite, hematite, etc. The U-Pb dating of detrital zircon generally indicates three age peaks, i.e., 260 similar to Ma, 1850 similar to Ma and 2450 similar to Ma, respectively. In conclusion, the source rocks may have been formed at active continental margins, e.g., in a continental margin arc environment. The sedimentary materials mainly come from khondalite series, TTGs, granulite, and mafic-ultramafic intrusive rocks distributed among the Daqing-Ula Mountains and adjacent areas, etc. The Late Paleozoic U-rich intermediate and acidic magmatic rocks spreading over the eastern part of the Ula-Daqing and Wolf mountains have provided the main uranium sources for the formation of major U deposits in the northern Ordos Basin.