In this paper, we present the new results of the U–Pb age dating and Lu-Hf isotopic analysis of detrital zircons of the four representative metasedimentary rock samples from the Mongol Altai Group, Mongolian part of the Altai-Mongolian terrane. Our new results indicate that the metasedimentary rocks of the Mongol Altai Group were formed after ∼497 Ma, Late Cambrian and deposited during the Early-Middle Ordovician. The detrital zircons of four samples yield a two major age peaks at 503–517 Ma, and 775–843 Ma, respectively, with minor involvement of older zircons. The nearby Lake Zone of Ikh-Mongol Arc most likely provided plenty of Early Paleozoic materials, the subdominant Neoproterozoic detrital zircons could be supplied by the felsic intrusions along the western margin of the Tuva-Mongol microcontinent, and the sparse older zircons may be derived from its basement. With combination of previous studies in the Chinese Altai, Russian Altai and Hovd terrane, our data suggest that the Altai–Mongolian terrane possibly represents a coherent continental arc-accretionary prism system built upon the active margin of the western Mongolia during the Cambrian to Ordovician. Moreover, the dominant Neoproterozoic to Early Paleozoic detrital zircons from the Mongol Altai sequence yield largely varied εHf(t) values from −17.4 to +12.0, indicating that input juvenile material and reworking of crustal components are both important in the accretionary orogenesis. A compilation of U–Pb and Hf isotope data of detrital zircons shows that the source area underwent two most extensive magmatic activities at ca. 470–574 Ma and 687–967 Ma, respectively.