Crustal‐scale imaging by the full‐waveform inversion (FWI) of long‐offset seismic data is inherently difficult because the large number of wavelengths propagating through the crust makes the inversion prone to cycle skipping. Therefore, efficient crustal‐scale FWI requires an accurate starting model and a stable workflow minimizing the nonlinearity of the inversion. Here we attempt to reprocess a challenging 2‐D ocean‐bottom seismometer (OBS) data set from the eastern Nankai Trough. The starting model is built by first‐arrival traveltime tomography (FAT), which is FWI assisted for tracking cycle skipping. We iteratively refine the picked traveltimes and then reiterate the FAT until the traveltime residuals remain below the cycle‐skipping limit. Subsequently, we apply Laplace‐Fourier FWI, in which progressive relaxation of time damping is nested within frequency continuation to hierarchically inject more data into the inversion. These two multiscale levels are complemented by a layer‐stripping approach implemented through offset continuation. The reliability of the FWI velocity model is assessed by means of source wavelet estimation, synthetic seismogram modeling, ray tracing modeling, dynamic warping, and checkerboard tests. Although the viscoacoustic approximation is used for wave modeling, the synthetic seismograms reproduce most of the complexity of the data with a high traveltime accuracy. The revised FWI scheme produces a high‐resolution velocity model of the entire crust that can be jointly interpreted with migrated images derived from multichannel seismic data. This study opens a new perspective on the design of OBS crustal‐scale experiments amenable to FWI; however, a further assessment of the optimal OBS spacing is required for reliable FWI.