Urban geophysical exploration plays an important role in the sustainable development of and the mitigation of geological hazards in metropolitan areas. However, it is not suitable to implement active seismic methods in densely populated urban areas. The rapidly developing ambient-noise tomography (ANT) method is a promising technique for imaging the near-surface seismic velocity structure. We selected the West Lake area of the city of Hangzhou as a case study to probe the shallow subsurface shear-wave velocity (Vs) structure using ANT. We conducted seismic interferometry on the ambient-noise data recorded by 28 seismograph stations during a time period of 17 days. Fundamental-mode Rayleigh-wave group- and phase-velocity dispersion data were measured from cross-correlation functions and then inverted for a 3D Vs model of the uppermost 1 km that covers an area of about 7 km × 8 km. The tomographic results reveal two prominent anomalies, with high velocities in the southwest and low velocities in the northeast. The fast anomaly corresponds to the presence of limestone and sandstone, whereas the slow anomaly is due to the relatively low-velocity rhyolite and volcanic tuff in the area. The boundary between the two anomalies lies to the NE of an NW–SE trending fault, indicating that the fault dips toward the NE. In addition, the pronounced low-velocity anomalies appear under the Baoshi mountain, likely due to the thick rhyolite and volcanic tuff beneath the extinct volcano. Our results correlate well with regional geological features and suggest that ANT could be a promising technique for facilitating the exploration of urban underground space.