The detailed studies of converted S-waves recorded on the Ocean Bottom Seismometer (OBS) can provide evidence for constraining lithology and geophysical properties. However, the research of converted S-waves remains a weakness, especially the S-waves’ inversion. In this study, we applied a travel-time inversion method of converted S-waves to obtain the crustal S-wave velocity along the profile NS5. The velocities of the crust are determined by the following four aspects: (1) modelling the P-wave velocity, (2) constrained sediments Vp/Vs ratios and S-wave velocity using PPS phases, (3) the correction of PSS phases’ travel-time, and (4) appropriate parameters and initial model are selected for inversion. Our results show that the vs. and Vp/Vs of the crust are 3.0–4.4 km/s and 1.71–1.80, respectively. The inversion model has a similar trend in velocity and Vp/Vs ratios with the forward model, due to a small difference with ∆Vs of 0.1 km/s and ∆Vp/Vs of 0.03 between two models. In addition, the high-resolution inversion model has revealed many details of the crustal structures, including magma conduits, which further supports our method as feasible.