CO2 mineralisation is a process that can store the CO2 as a solid mineral permanently, to mitigate carbon emissions. Brines rich in alkaline earth metals present an attractive opportunity to trap CO2 in the form of insoluble carbonates. Moreover, this can be accomplished, as shown in this work, using flue gas concentrations of CO2 and at nearambient temperatures, eliminating the need for energy-intensive CO2 capture step and heating of dilute aqueous solutions. The conventional alkaline substances to neutralise the solution, such as sodium hydroxide or amines, are costly, and the processes required to regenerate them (e.g. distillation or electrolysis) are energy intensive, which hinders the feasibility of this CO2 sequestration approach. We herein developed a process to remove chloride anions from alkaline brines by ion exchange, using lamellar structured materials, namely hydrotalcites (HT).These HT, which are layered double hydroxides prepared by co-precipitation method, release hydroxyl groups in exchange for chloride, sufficiently raising the pH of brines to enable the precipitation of carbonates during CO2 mineralisation. Several calcined-HT were synthesized using different ratios of magnesium and aluminium content, and various reaction temperatures and solid-to-liquid ratios were investigated for chloride removal. Moreover, the HT materials are recyclable for multiple usage by taking advantage of the HT's 'memory effect' property.Gaseous CO2 and Na2CO3 solution were tested as the recharging agents, to replace the chloride anions from the spent HT interlayers and intercalate with HCO3or CO3 2-, followed by a calcination process to produce the reusable calcined-HT. Several reaction cycles were conducted to evaluate the reusable property. It was found that the chloride removal efficiency remains over 70% after five cycles, and calcium utilisation efficiency of the brine carbonation process can surpass 90%. This unique cyclical closed-loop HT process thus presents a more cost-and energy-effective approach to brine carbonation than previous studies. In addition, the produced carbonates are of sufficient quality for a variety of applications that can further reduce the process cost of this type of CO2 sequestration.