The research presented here investigates the reaction mechanism of wollastonite in situ mineral carbonation for carbon dioxide (CO2) sequestration. Because wollastonite contains high calcium (Ca) content, it was considered as a suitable feedstock in the mineral carbonation process. To evaluate the reaction mechanism of wollastonite for geological CO2 sequestration (GCS), a series of carbonation experiments were performed at a range of temperatures from 35 to 90 °C, pressures from 1500 to 4000 psi, and salinities from 0 to 90,000 mg/L NaCl. The kinetics batch modeling results were validated with carbonation experiments at the specific pressure and temperature of 1500 psi and 65 °C, respectively. The results showed that the dissolution of calcium increases with increment in pressure and salinity from 1500 to 4000 psi and 0 to 90000 mg/L NaCl, respectively. However, the calcium concentration decreases by 49%, as the reaction temperature increases from 35 to 90 °C. Besides, it is clear from the findings that the carbonation efficiency only shows a small difference (i.e., ±2%) for changing the pressure and salinity, whereas the carbonation efficiency was shown to be enhanced by 62% with increment in the reaction temperature. These findings can provide information about CO2 mineralization of calcium silicate at the GCS condition, which may enable us to predict the fate of the injected CO2, and its subsurface geochemical evolution during the CO2-fluid-rock interaction.