Daluoshan Mountain lies at the leading edge of the arcuate tectonic belt at the northeastern margin of the Tibetan Plateau, and is the landform boundary zone between the active Tibetan Plateau and the stable North China Craton. Understanding the late Cenozoic uplift of Daluoshan is important for discussing the expansion of the arcuate tectonic belt of the northeastern margin of the Tibetan Plateau and its influence on the western North China Craton. In this study, the late Cenozoic uplift of Daluoshan is reconstructed from the development of the late Cenozoic alluvial fan around Daluoshan. The entire sedimentary sequence and framework of the fan was reconstructed on the basis of the newly obtained drilling data. The initial timing of the late Cenozoic uplift of Daluoshan and the key stages of uplift during the Pleistocene were reconstructed using cosmogenic nuclide, optically stimulated luminescence, and detrital zircon U–Pb dating analyses. The late Cenozoic alluvial fan at the front of Daluoshan overlies a set of fluvial-facies strata; therefore, the commencement of alluvial-fan development marks the start of the late Cenozoic uplift of Daluoshan. The timing of this event can be constrained to 4.64 Ma. The main gravel type at the base of the Daluoshan fan is Carboniferous purple sandstone, and there is a gradual upward transition to gravel clasts of slightly metamorphosed grayish-black argillaceous siltstone of the Ordovician Miboshan Formation, indicating that Carboniferous strata were exposed on Daluoshan during the initial stage of the late Cenozoic uplift. Two extensive gravel layers (dated to 0.76–0.6 and 0.05 Ma) developed during the Pleistocene, indicating two episodes of considerable uplift. This study provides a new time scale for the uplift and expansion of the arcuate tectonic belt at the northeastern margin of the Tibetan Plateau.