The structure, composition, and age of Vendian–Early Cambrian plagiogranitoid associations composing the Kshta and Taraskyr massifs of the Yenisei pluton in the Altai–North Sayan island-arc belt are considered. We have established that these associations formed within 550–520 Ma and differ in petrographic composition and sources. Two stages of island-arc plagiogranitoid magmatism are recognized: early (550–540 Ma, formation of plagiogranitoids of the Kshta (545 ± 8 Ma) and Taraskyr (545 ± 7 Ma) massifs) and late (525–520 Ma, formation of plagiogranitoids of the Maina complex of the Yenisei (524 ± 2 Ma) and Tabat plutons). By petrochemical composition and geochemical characteristics, the rocks of the Kshta massif are high-alumina plagiogranitoids similar to adakites. They might have been produced through the melting of metabasites compositionally similar to N-MORB in equilibrium with garnet-containing restite during the subduction of oceanic slab at ≥ 15 kbar. The rocks of the Taraskyr massif are low-alumina plagiogranites. They formed through the melting of metabasites located in the lower layers and(or) the basement of the island-arc system in equilibrium with plagioclase-containing restite at 3–8 kbar. The low-alumina plagiogranitoids of the Yenisei pluton melted out under the same conditions. Isotope-geochemical studies showed that the Vendian–Early Cambrian plagiogranitoids formed at the early stage are characterized by high positive ∑ Nd(T) values (7.5–4.9), Late Riphean model Nd-age (TNd(DM) = 0.64–0.98 Ga), and Sr isotope ratio varying from 0.7040 to 0.7053. These data point to the juvenile parental melts of the rocks and the varying content of ancient crustal material in the magma generation zone.