Mineral carbonation incurs high operating costs, as large amounts of chemicals and energy must be used in the process. Its implementation on an industrial scale requires reducing expenditures on chemicals and energy consumption. Thus, this work aimed to investigate the significant factors involved in pH-swing mineral carbonation and their effects on CO2 capture efficiency. A central composite rotatable design (CCRD) was employed for optimizing the operational parameters of the acid dissolution of serpentinite. The results showed that temperature exerts a significant effect on magnesium dissolution. By adjusting the reaction temperature to 100 °C and setting the hydrochloric acid concentration to 2.5 molar, 96% magnesium extraction was achieved within 120 min of the reaction and 91% within 30 min of the reaction. The optimal efficiency of carbon dioxide capture was 40–50%, at higher values than those found in literature, and 90% at 150 bar and high pressures. It was found that it is technically possible to reduce the reaction time to 30 min and maintain magnesium extraction levels above 90% through the present carbonation experiments.