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Fast water transport channels are crucial for waterrelated membrane separation processes.However,overcoming the trade-off between flux and selectivity is still am ajor challenge.T oa ddress this,w ec onstructed spherical polyelectrolyte brush (SPB) structures with ah ighly hydrophilic polyelectrolyte brush layer,a nd introduced them into GO laminates,w hichi ncreased both the flux and the separation factor.A t7 0 8 8C, the flux reached 5.23 kg m À2 h À1 ,a nd the separation factor of butanol/water increased to % 8000, which places it among the most selective separation membranes reported to date.I nterestingly,f urther studies demonstrated that the enhancement of water transport was not only dependent on the hydrophilicity of the polyelectrolyte chains, but also influenced by their flexibility in the solvent. Quartz crystal microbalance with dissipation and molecular dynamics simulations revealed the structure-performance correlations between water molecule migration and the flexibility of the ordered polymer chains in the 2D confined space.