Artificial membranes with ion-selective nanochannels for high-efficiency mono/divalent ion separation are of great significance in water desalination and lithium-ion extraction, but they remain a great challenge due to the slight physicochemical property differences of various ions. Here, the successful synthesis of two-dimensional TpEBr-based covalent organic framework (COF) nanosheets, and the stacking of them as consecutive membranes for efficient mono/divalent ion separation is reported. The obtained COF nanosheet membranes with intrinsic one-dimensional pores and abundant cationic sites display high permeation rates for monovalent cations (K