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Abstract: As the main factor influencing the flow and preservation of underground fluids, wettability has a profound impact on CO2 sequestration (CS). However, the influencing factors and internal interaction mechanisms of shale kerogen wettability remain unclear. In this study, we used molecular dynamics to simulate the influence of temperature, pressure, and salinity on wettability. Furthermore, the results were validated through various methods such as mean square displacement, interaction energy, electrostatic potential energy, hydrogen bonding, van der Waals forces, and electrostatic forces, thereby confirming the reliability of our findings. As temperature increases, water wettability on the surface of kerogen increases. At CO2 pressures of 10 and 20 MPa, as the temperature increases, the kerogen wettability changes from CO2 wetting to neutral wetting. As the CO2 pressure increases, the water wettability on the surface of kerogen weakens. When the pressure is below 7.375 MPa and the temperature is 298 or 313 K, kerogen undergoes a wettability reversal from neutral wetting to CO2 wetting. As salinity increases, water wettability weakens. Divalent cations (Mg2+ and Ca2+) have a greater impact on wettability than monovalent cations (Na+). Water preferentially adsorbs on N atom positions in kerogen. CO2 is more likely to form hydrogen bonds and adsorb on the surface of kerogen than H2O. As the temperature increases, the number of hydrogen bonds between H2O and kerogen gradually increases, while the increase in pressure reduces the number of hydrogen bonds. Although high pressure helps to increase an amount of CS, it increases the permeability of a cap rock, which is not conducive to CS. Therefore, when determining CO2 pressure, not only a storage amount but also the storage safety should be considered. This research method and results help optimize the design of CS technology, and have important significance for achieving sustainable development.