Efficient lithium extraction from salt lakes is essential for a sustainable resource supply. This study tackles the challenge of separating Li+ from Mg2+ in complex brines by innovatively integrating two-dimensional (2D) graphene oxide (GO) with bimetallic metal-organic frameworks (MOFs). Zn2+ and Co2+ ions are confined within GO interlayers through an in situ synthesis, forming a 2D Zn-Co MOFs/GO membrane (Zn-Co-GOM). This design exploits the unique advantages of bimetallic MOFs, including enhanced structural stability and superior ion separation capabilities due to the synergistic effects of Zn and Co. The Zn-Co-GOM demonstrates an impressive separation factor of 191 for Li+ over Mg2+, significantly surpassing traditional membranes. This exceptional selectivity is achieved through a combination of size exclusion effects and ion transport energy barriers. Our approach not only enhances the practical application of membrane technology for lithium extraction from salt lakes but also provides valuable insights into the underlying separation mechanisms.