A multioffset, three‐component vertical seismic profiling (VSP) experiment was carried out in the Sudbury Basin, Ontario, as a part of the LITHOPROBE Sudbury Transect. The main objectives were determination of the shallow velocity structure in the middle of the Sudbury Basin, development of an effective VSP data processing flow, correlation of the VSP survey results with the surface seismic reflection data, and demonstration of the usefulness of the VSP method in a crystalline rock environment. The VSP data processing steps included rotation of the horizontal component data, traveltime inversion for velocity analysis, Radon transform for wavefield separation, and preliminary analysis of shear‐wave data. After wavefield separation, the flattened upgoing wavefields for both P‐waves and S‐waves display consistent reflection events from three depth levels. The VSP-CDP transformed section and corridor stacked section correlate well with the high‐resolution surface reflection data. In addition to obtaining realistic velocity models for both P‐ and S‐waves through least‐square inversion and synthetic seismic modeling for the Chelmsford area, the VSP experiment provided an independent estimation for the reflector dip using three component hodogram analysis, which indicates that the dip of the contact between the Chelmsford and Onwatin formations, at an approximate depth of 380 m in the Chelmsford borehole, is approximately 10.5° southeast. This study demonstrates that multioffset, three‐component VSP experiments can provide important constraints and auxiliary information for shallow crustal seismic studies in crystalline terrain. Thus, the VSP technique bridges the gap between the surface seismic‐reflection technique and well‐log surveys.