Daluo Mountains lie at front of the arcuate tectonic belt at the northeastern margin of the Tibetan Plateau, and are the landform boundary zone between the active Tibetan Plateau and the stable North China Craton. Studying of the late Cenozoic uplift evolution of Daluo Mountains is important for understanding the expansion mechanism 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 Daluo Mountains is constructed from the development of the late Cenozoic alluvial fan around Daluo Mountains. The entire sedimentary sequence and framework of the fan was revealed by the newly obtained drilling core data. The cosmogenic nuclide, optically stimulated luminescence, and detrital zircon U-Pb dating results provide new evidences for discussion about the initial timing of the late Cenozoic uplift of Daluo Mountains and the key stages of uplift during the Pleistocene. The late Cenozoic alluvial fan at front of Daluo Mountains overlies a set of fluvial-facies strata; therefore, development of the alluvial-fan marks the start of late Cenozoic uplift of Daluo Mountains. The timing of this event can be constrained to ~4.64 Ma. Two extensive gravel layers (dated to ca. 0.76–0.6 Ma 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.