The Late Carboniferous–Early Permian period is a significant transitional phase within the late Paleozoic ice age and to investigate the sedimentary–tectonic evolution of the Qaidam Basin in this period is crucial for comprehensively understanding the tectonic history of the northeastern Paleo-Tethys Ocean and the related response to energy and mineral resources. This paper focuses on the Carboniferous–Permian strata of the Wanggaxiu-Dongdagou outcrop that was taken to represent the southern Oulongbruk terrane in the eastern Qaidam Basin. We determined the ages of tuff interbeds within the Zhabusagaxiu Formation originally identified as the upper Carboniferous and obtained the crystallization age spectra of detrital zircon grains from Carboniferous to lower Permian sandstones using laser ablation inductively coupled plasma mass spectrometry (LA-ICP-MS) isotope geochemical techniques. The origin of the volcanic ash and the sedimentary–tectonic evolution in this period were analyzed. The results indicate that the original Zhabusagaxiu Formation can be divided into two chronostratigraphic units: the upper Carboniferous Zhabusagaxiu Formation and the lower Permian. The earliest age obtained from tuffaceous layers within the dark shale interval is 297.8 ± 3.0 Ma (mean square weighted deviation (MSWD) = 0.87), which suggests a stratigraphic boundary between the Carboniferous and Permian periods. Detrital zircons from Carboniferous–Permian samples in the southern Oulongbruk terrane predominantly originated from the Qaidam block-North Qaidam ultrahigh-pressure belt continental island arc to the south. The ultrahigh-pressure belt had a significantly increased contribution to the detrital source supply system from the Late Carboniferous to Early Permian, while the Qaidam block experienced frequent volcanic eruptions from 298 to 293 Ma, dispersing volcanic ash only northward to the Oulongbruk back-arc basin and the Zongwulong Trough. The upper Carboniferous Zhabusagaxiu Formation was marked by siliceous clastic rock–carbonate rock interbedding in an epicontinental sea, while the lower Permian was characterized by shallow to bathyal marine shelf to subaqueous sedimentation. The Early Permian transgression potentially represents the largest transgression during the late Paleozoic ice age, indicating an enriched hydrocarbon-generating interval.