The preparation of Li₂CO₃ from brine with a high mass ratio of Mg/Li is a worldwide technology problem. Membrane separation is considered as a green and efficient method. In this paper, a comprehensive Li₂CO₃ preparation process, which involves electrochemical intercalation-deintercalation, nanofiltration, reverse osmosis, evaporation, and precipitation, was constructed. Concretely, the electrochemical intercalation-deintercalation method shows excellent separation performance of lithium and magnesium, and the mass ratio of Mg/Li decreased from the initial 58.5 in the brine to 0.93 in the obtained lithium-containing anolyte. Subsequently, the purification and concentration are performed based on nanofiltration and reverse osmosis technologies, which remove mass magnesium and enrich lithium, respectively. After further evaporation and purification, industrial-grade Li₂CO₃ can be prepared directly. The direct recovery of lithium from the high Mg/Li brine to the production of Li₂CO₃ can reach 68.7%, considering that most of the solutions are cycled in the system, the total recovery of lithium will be greater than 85%. In general, this new integrated lithium extraction system provides a new perspective for preparing lithium carbonate from high Mg/Li brine.