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Mineral dehydration in the subduction zone enormously affects Earth’s geodynamics and the global geochemical cycles of elements. This work uses Raman spectroscopy and X-ray diffraction to investigate the dehydration process of antigorite under compression and shear loading conditions in a rotational diamond anvil cell (RDAC) at room temperature. In order to compare the shear effects, T301 stainless steel and Kapton plastic are applied as the gasket materials. In the experiment using a high-strength T301 stainless steel gasket, two new broad OH-stretching peaks of H₂O and H₃O₂⁻ appear at 3303 and 3558 cm⁻¹, respectively, at 1.7 GPa. The original sharp OH-stretching peaks of antigorite at 3668 and 3699 cm⁻¹ remain, while the central pressure is increased to 8.0 GPa, and the largest pressure gradient is about 2.5 GPa in the sample chamber. In another experiment with a low-strength gasket of Kapton plastic, two new OH-stretching broad peaks of H₂O and H₃O₂⁻ also start to appear at 3303 and 3558 cm⁻¹, respectively, at a lower pressure of 0.3 GPa, but the original sharp OH-stretching peaks of antigorite at 3668 and 3699 cm⁻¹ almost completely vanish as the central pressure reaches 3.0 GPa, with the largest pressure gradient at around 4.8 GPa. The comparison between the two experiments shows that antigorite is easier to dehydrate in the chamber of a Kapton plastic gasket with a larger gradient of shear stress. However, its axial compression stress is lower. The high-pressure Raman spectra of MgO₂(OH)₄ octahedron and SiO₄ tetrahedron in the low wavenumber zones (100–1200 cm⁻¹) combined with the micro-beam X-ray diffraction spectrum of the recovered product strongly support the structural breakdown of antigorite. This investigation reveals that the water-bearing silicate minerals have strong shear dehydration in the cold subduction zone of the plate, which has important applications in predicting the physical and chemical properties of subduction zones and deducing the rate of plate subduction.