New seismic data from marine air-gun and Vibroseis profiles in Lake Ontario and Lake Erie provide images of subhorizontal Phanerozoic sediments underlain by a remarkable series of easterly dipping reflections that extends from the crystalline basement to the lower crust. These reflections are interpreted as structural features of crustal-scale subdivisions within the Grenville Orogen. Broadly deformed, imbricated, and overlapping thrust sheets within the western Central Metasedimentary Belt are succeeded to the west by a complex zone of easterly dipping, apparent thrust faults that are interpreted as a southwest subsurface extension of the boundary zone between the Central Metasedimentary Belt and the Central Gneiss Belt. The interpreted Central Metasedimentary Belt boundary zone has a characteristic magnetic anomaly that provides a link from the adjacent ends of lakes Ontario and Erie to structures exposed 150 km to the north. Less reflective, west-dipping events are interpreted as structures within the eastern Central Gneiss Belt. The seismic interpretation augments current tectonic models that suggest the exposed ductile structures formed at depth as a result of crustal shortening along northwest-verging thrust faults. Relatively shallow reflections across the boundary region suggest local, Late Proterozoic extensional troughs containing post-Grenville sediments, preserved possibly as a result of pre-Paleozoic reactivation of basement structures.