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Abstract Abundant Li resources in the ocean are promising alternatives to refining ore, whose supplies are limited by the total amount and geopolitical imbalance of reserves in Earth's crust. Despite advances in Li⁺extraction using porous membranes, they require screening other cations on a large scale due to the lack in precise control of pore size and inborn defects. Herein, MoS₂nanoflakes on a multilayer graphene membrane (MFs‐on‐MGM) that possess ion channels comprising i) van der Waals interlayer gaps for optimal Li⁺extraction and ii) negatively charged vertical inlets for cation attraction, are reported. Ion transport measurements across the membrane reveal ≈6‐ and 13‐fold higher selectivity for Li⁺compared to Na⁺and Mg²⁺, respectively. Furthermore, continuous, stable Li⁺extraction from seawater is demonstrated by integrating the membrane into a H₂and Cl₂evolution system, enabling more than 10⁴‐fold decrease in the Na⁺concentration and near‐complete elimination of other cations.