Field investigations in the western part of the Cape Smith Belt outlined four fault-bounded lithological assemblages tectonically overlying foliated to gneissic granitoids of the Archean Superior Province. These assemblages comprise sequences of pillowed volcanic rocks, sedimentary rocks of pelitic and psammitic composition, and volcaniclastic rocks. They are juxtaposed along the Lanyan Lake Fault against a structurally thickened sequence of mafic to ultramafic pillowed volcanic suite belonging to the Chukotat Group. The occurrence of volcaniclastic horizons in the uppermost levels of the Chukotat Group may indicate a northward facies transition from sea-floor volcanism to arc sedimentation, the latter corresponding to the Parent Group. A major pluton intruding the upper Chukotat Group, if assigned to the younger Narsajuaq intrusive suite, provides support for an 1844 – 1826 Ma link between two tectonic domains, formerly considered "suspect." These domains lie on either side of the Bergeron Fault in the east and central parts of the Cape Smith Belt. This fault, formerly interpreted as extending to Hudson Bay, was not recognized in this work. Thrust faulting, involving three kilometre-thick imbricate slices enclosing the Superior Province, was followed by the development of the Cape Smith Synclinorium with overturning of its northern limb, forelimb faulting, and large-scale folding along northwest-trending axes.