We present new data on geochemistry, isotopic geochemistry, and geochronology of the Early Cambrian igneous rocks of the northeastern Siberian Craton (Kharaulakh anticlinorium, contact between the Siberian Platform and the West Verkhoyansk sector of the Verkhoyansk fold-and-thrust belt united into an Early Cambrian bimodal complex. This complex comprises trachyrhyolites forming pebbles in conglomerates near the base of the Cambrian succession, overlying trachybasalts, and mafic sills and dikes cutting Neoproterozoic strata. According to chemical composition, the felsic rocks are high-alkali rhyolites and correspond to A-type granites. The high contents of Ta, Nb, Hf, Tb, and Zr in these rocks suggest the presence of enriched mantle material in their magmatic sources. The mafic volcanics are high-Ti trachybasalts and trachydolerites with similar geochemical characteristics corresponding to alkali basalts or OIB. The high (Tb/Yb)PM ratios in these volcanics evidence that their magmatic source was the garnet peridotite mantle located at depths more than 90 km and characterized by a low degree of melting. However, the rhyolites, trachybasalts, and trachydolerites show high positive εNd(T) values (4.2–4.7, 7.5–8.9, and 7.2–8.2, respectively) indicating a depleted mantle source and no crustal contamination. The high (Nb/Yb)PM ratio points to the mixing of magmas from enriched and depleted mantle sources. Mafic magmas might have been generated from a heterogeneous source or interacted with the depleted mantle before intrusion. Both the felsic and the mafic rocks formed in within-plate environments. U–Pb zircon dating yielded concordant ages of 525.6 ± 3.9 and 537.0 ± 4.2 Ma, corresponding to the Early Cambrian age of the rhyolites. The date of 546.0 ± 7.7 Ma obtained for one sample points (with regard to the error) to the Late Vendian–Early Cambrian age. Thus, at the Vendian–Early Cambrian boundary, the northeastern Siberian Platform was subjected to continental rifting accompanied by bimodal magmatism of antidrome evolution. According to paleotectonic reconstructions, this part of the Siberian Craton might have been connected with the eastern margin of Laurentia in the Late Neoproterozoic (Late Riphean–Late Vendian), and continental rifting that started at the Vendian–Cambrian boundary led to their separation. The obtained isotope-geochronological data suggest that the studied bimodal complex began to form at the Vendian–Cambrian boundary and this process terminated no earlier than the end of the Terreneuvian (Tommotian), i.e., the complex formed during rifting for about 20 Myr.