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In the last two years, the rapidly rising demand for lithium has exceeded supply, resulting in a sharp increase in the price of the metal. Conventional electric driven membrane processes can separate Li⁺ from divalent cations, but there is virtually no commercial membrane that can efficiently and selectively extract Li⁺ from a solution containing chemically similar ions such as Na⁺ and K⁺. Here, we show that the different movement behavior of Li⁺ ion within the sub-nanometre channel leads to Li⁺ ion-selectivity and high transport rate. Using inexpensive negatively charged 2D subnanometer hydrous phyllosilicate channels with interlayer space of 0.43 nm in a membrane-like morphology, we observed that for an interlayer spacing of below 1 nm, Li⁺ ions move along the length of the channel by jumping between its two walls. However, for above 1 nm spacing, the ions used only one channel wall to jump and travel …