Within the diamond anvil cell, the Raman spectroscopic study of serpentine was operated at room temperature and under pressures from 1 atm to 5 140 MPa. This study analyzed the pressure dependence of the low-frequency Raman vibrational modes of sepentine at 388, 471, 692 and 705 cm-1 respectively. The vibrational modes of inner OH groups at 3 664 cm-1 and inter-layer OH groups at 3 696 cm-1 shifted linearly with the increasing pressures. The pressure-related slope of 3 664 cm-1 was 3.3 cm-1·GPa-1. The vibrational mode at 3 696 cm-1 of the inter-layer hydroxyl shifted upwards with the pressure-related slope 8.3 cm-1·GPa-1 up to 2.0 GPa, and then with 1.1 cm-1·GPa-1 from 2.0 GPa to ca. 5.0 GPa. It could be interpreted that the hydrogen bond of the inter-layer hydroxyl made dominant contribution to such experimental phenomena. In addition, the dehydration of serpentine did not occur under such conditions.