Origins of early Paleozoic metabasites (granulites and amphibolites) and their host metasedimentary rocks in the Dunhuang block, NW China, are addressed by new geochronological and geochemical data. The metabasites show back-arc basalt–like geochemical features, marked by high Zr/Nb ratios and Zr-Hf troughs, but they can be classified into two groups based on their dissimilar protolith ages and distinct Nd signatures. Most group I metabasaltic rocks were emplaced before 455 Ma and possess high Ba/Nb ratios (11.46–224), low (Nb/La)PM (0.10–0.71), and negative whole-rock εNd(t) values (−12.7 to −2.7), whereas group II rocks have protolith ages around 445 Ma, low Ba/Nb ratios (0.70–22.93), low (Nb/La)PM (0.78–1.51), and less evolved whole-rock Nd isotopic features (εNd[t]: −2.0 to +2.7). It is proposed that group I metabasites originated from an enriched lithospheric mantle, while group II metabasites were derived from the depleted asthenospheric mantle. The metasedimentary rocks received detritus mainly from the neighboring Cambrian magmatic arc, and they are compositionally similar to active-margin sediments. Metamorphic zircon U-Pb ages ranging 462–422 Ma from the investigated rocks together with prominent magmatism further suggest high-grade metamorphism prevailing during the Late Ordovician–early Silurian. Based on these data, a Cascadia-type evolution is proposed involving an Ordovician–early Silurian suprasubduction stretching of the Cambrian active continental margin, which culminated with mantle upwelling. Recent paleogeographic reconstructions support the evolution and assembly of interior Proto–Tethys-Ran oceanic and continental plates, including the Dunhuang block, between 510 and 440 Ma, followed by Panthalassan subduction beneath the Tarim–North China continental assemblage at 440–430 Ma.