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This study presents an approach to better characterize the P‐wave and S‐wave velocity structure of the seafloor sediment layer using ocean bottom seismometers. The presence of low‐velocity seafloor sediment layers influences the observed seismic record at the seafloor over a broad frequency range, such that detailed knowledge of this sediment structure is essential to predict its effect on teleseismic records. We use the radial component of teleseismic P waves and autocorrelation functions of the radial, vertical, and pressure components of teleseismic P and S waves to obtain sediment layer models using the Markov chain Monte Carlo approach with parallel tempering. Synthetic tests show that the body waves constrain the P‐ and S‐wave impedances and travel times and the P‐ to S‐wave velocity ratio of the sediment layers. The proposed method resolves thin layers at a high resolution, including the uppermost thin (∼50 m to a few hundred meters) low S‐wave velocity layer. Real data applications at sites across the Pacific Ocean that are coincident with previous in situ studies demonstrate the effectiveness of this method in characterizing the seafloor sediment unit. The sediment models characterized by this new approach will allow us to more accurately predict and correct the effects of sediment layers in generating P‐ and S‐wave reverberations. Plain Language Summary: Ocean bottom seismometers are powerful tools for investigating the detailed structure of the oceanic mantle. However, most ocean bottom seismometers are placed above the low‐velocity water‐saturated sediment layer, such that their seismic records are inevitably affected by this seafloor sediment layer. Detailed constraints on the structure of the seafloor sediment layer allow us to accurately predict its effects on the observed seismic records. The seafloor sediment layer may consist of multiple discontinuities and vary regionally. This study proposes a new approach for characterizing the seismic properties of the seafloor sediment layer using teleseismic body waves recorded at ocean bottom seismometers. Synthetic tests show that the method can resolve thin sublayers within the sediment layer, such as a very thin low shear‐wave velocity layer and sharp seismic velocity jumps. Real data applications show that the sediment models obtained using this approach are in good agreement with those obtained from direct measurements and previous body‐wave analyses. Our proposed method will enable more detailed prediction and correction of the influence of the sediment layer on ocean bottom seismometer records, thereby providing more accurate constraints on deeper Earth structures. Key Points: The seismic properties of the seafloor sediment layer are characterized using ocean bottom seismometer teleseismic body‐wave recordsThe P‐ and S‐wave impedances and travel times and the VP/VS values of each sublayer within the sediment layer are resolvedIn situ seafloor sediment structure constraints will enable accurate correction and prediction of shallow structure effects [ABSTRACT FROM AUTHOR]