The Nemiscau subprovince is a metasedimentary rocks-dominated sequence of the Archean eastern Superior Province. It is bounded by the gneissic and tonalite-trondhjemite-granodiorite (TTG) rocks-dominated La Grande and Opatica subprovinces. The Nemiscau consists of variably migmatized metasedimentary rocks and felsic to intermediate gneisses and plutonic suites. Mafic-to-ultramafic metavolcanic rocks occur along its northern and southern boundaries. Previous structural and metamorphic studies suggested that it was the result of subduction-related, accretionary and collisional tectonics with adjacent plutonic terranes during the Kenorean orogeny. This study integrates various sets of structural, metamorphic, and U-Pb geochronological data suggesting a long-lasting tectonometamorphic evolution between ca. 2843 and 2598 Ma. Four tectonometamorphic events have been recognized. The first event (D1) is only locally preserved and occurred shortly after the deposition of the oldest volcanic sequences of the Nemiscau ( ca. 2756–2736 Ma) under amphibolite facies metamorphic conditions (M1). The kinematic analysis of shear zones bounding the supracrustal sequences of both the Nemiscau and La Grande subprovinces suggests their relative crustal sinking as compared to TTG of the La Grande and Opatica subprovinces, shortly after deposition (at ≤2724 and ≤2706 Ma, respectively). Sedimentation was followed by regional dip-slip-dominated (D2) deformation between ca. 2704 and 2671 Ma, coeval with extensive high-grade granulite facies metamorphism (M2) and anatexis in the Nemiscau subprovince from ca. 2697 to 2685 Ma, followed by exhumation between ca. 2677 and 2671 Ma. This D2 event was followed by regional-scale dextral strike-slip shearing (D3) from ca. 2658 until 2621 Ma at amphibolite facies metamorphism (M3). The youngest deformation event, D4, was accompanied by strain localization along brittle-to-ductile conjugated shear zones and waning crustal cooling from amphibolite to greenschist facies conditions at ca. 2598 Ma and younger. It is suggested that the Nemiscau, La Grande, and Opatica subprovinces represent a single composite terrane, and that their mutual boundaries do not correspond to “collisional sutures” between different crustal blocks or microcontinents. The Nemiscau subprovince is interpreted as a sedimentary sequence unconformably overlying a ca. 2760–2756 Ma (and older) basement made up of volcanic and crosscutting TTG. In terms of tectonic evolution, the overall structural architecture and isotopic ages of the Nemiscau, La Grande, and Opatica subprovinces support a tectonic model in which the vertical transfer of crustal material occurred during the early stages (D2) of regional deformation, which evolved into a predominant lateral crustal flow of the ductile crust during later stages (D3–D4). A non-uniformitarian tectonic model for the Archean more adequately accounts for synchronous vertical and horizontal tectonism as preserved in the Nemiscau basin.