Abstract We propose a new waveform inversion method to estimate the 2D S-wave velocity structure of deep sedimentary layers using broadband Love waves. As a preprocessing operation in our inversion scheme, we decompose earthquake observation records into velocity waveforms for periods of 1 s each. Then, we include in the inversion only those periods for which the assumption of 2D propagation holds, which we propose to determine through a principal component analysis. A linearized iterative inversion analysis for the selected Love wave segments filtered for periods of 1 s each allows a detailed estimation of the boundary shapes of interfaces over the seismic bedrock with an S-wave velocity of approximately 3 km/s. We demonstrate the effectiveness of the technique with applications to observed seismograms in the Kanto Plain, Japan. The differences between the estimated and existing velocity structure models are remarkable at the basin edges. Our results show remarkable differences from previous existing structural models, particularly near the basin edges while being in good agreement with the surface geology. Since a subsurface structure at a basin edge strongly affects the earthquake ground motions in a basin with the generation of surface waves, our method can provide a detailed model of a complex S-wave velocity structure at an edge part for strong ground motion prediction.