The Chukchi Borderland, a prominent bathymetric feature within the Arctic Ocean, has been interpreted as a fragment of an undeformed continental platform sequence rifted from the passive margin of Arctic Canada. Dredges collected for the U.S. Extended Continental Shelf project aboard the icebreaker U.S. Coast Guard Cutter Healy (cruise number HLY0905) recovered hundreds of kilograms of broken crystalline basement lithologies consisting of mylonitically deformed biotite-bearing amphibolite, garnet-bearing feldspathic gneiss, and augen-bearing orthogneiss from the Chukchi Borderland. Metamorphic zircon within the amphibolite and associated leucogranitic seams within these rocks yielded U-Pb zircon ages between ca. 480 and 530 Ma. Garnet-bearing feldspathic gneisses contain variably discordant Mesoproterozoic zircon, ca. 600 Ma igneous zircon, and ca. 485–505 Ma metamorphic overgrowths. While we interpret these gneisses as deformed and metamorphosed granitoids, they could, instead, have a very immature sedimentary protolith. The youngest rocks sampled were K-feldspar augen orthogneisses that yield ca. 430 Ma zircon crystallization ages. Whole-rock geochemistry and Sr-Nd isotopic data indicate that the orthogneisses are I-type calc-alkaline granitoids. All of the basement rocks including the orthogneisses are variably metamorphosed and mylonitized. Collectively, the U-Pb age, geochemistry, and fabric of the dredged Chukchi Borderland basement samples indicate that they represent Neoproterozoic–Ordovician orogenic crust and Silurian arc batholithic rocks. This geologic origin is inconsistent with the Neoproterozoic to early Paleozoic passive margin history of western Arctic Canada to which the Chukchi Borderland has been previously correlated. We alternatively propose that the basement of the Chukchi Borderland is related to the peri-Laurentian composite terranes of Pearya and western Svalbard that have similar geologic histories.