Crust and upper-mantle structure interpreted from wide-angle seismic data along a 260 km profile across the Central Metasedimentary Belt of the southern Grenville Province in Ontario and New York State shows (i) relatively high average crustal and uppermost mantle velocities of 6.8 and 8.3 km/s, respectively; (ii) east-dipping reflectors extending to 24 km depth in the Central Metasedimentary Belt; (iii) weak lateral velocity variations beneath 5 km; (iv) a mid-crustal boundary at 27 km depth; and (v) a depth to Moho of 43–46 km. The wide-angle model is generally consistent with the vertical-incidence reflectivity of an intersecting Lithoprobe reflection line. The mid-crustal boundary correlates with a crustal detachment zone in the Lithoprobe data and the depth extent of east-dipping wide-angle reflectors. Regional structure and aeromagnetic anomaly trends support the southwest continuity of Grenville terranes and their boundaries from the wide-angle profile to two reflection lines in Lake Ontario. A zone of wide-angle reflectors with an average apparent eastward dip of 13° has a surface projection that correlates spatially with the boundary between the Elzevir and Frontenac terranes of the Central Metasedimentary Belt and resembles reflection images of a crustal-scale shear zone beneath Lake Ontario. A high-velocity upper-crustal anomaly beneath the Elzevir–Frontenac boundary zone is positioned in the hanging wall associated with the concentrated zone of wide-angle reflectors. The high-velocity anomaly is coincident with a gravity high and increased metamorphic grade, suggesting northwest transport of mid-crustal rocks by thrust faulting consistent with the mapped geology. The seismic data suggest (i) a reflective, crustal-scale structure has accommodated northwest-directed tectonic transport within the Central Metasedimentary Belt; (ii) this structure continues southwest from the exposed Central Metasedimentary Belt to at least southern Lake Ontario; and (iii) crustal reflectivity and complexity within the eastern Central Metasedimentary Belt is similar to that observed at the Grenville Front and the western Central Metasedimentary Belt boundary.