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The attainment of carbon neutrality requires the development of aqueous energy conversion and storage devices. However, these devices exhibit limited performance due to the permeability–selectivity trade-off of permselective membranes as core components. Herein, we report the application of a synergistic approach utilizing two-dimensional nanoribbons-entangled nanosheets to rationally balance the permeability and selectivity in permselective membranes. The nanoribbons and nanosheets can be self-assembled into a nanofluidic membrane with a distinctive “island-bridge” configuration, where the nanosheets serve as isolated islands offering adequate ionic selectivity owing to their high surface charge density, meanwhile bridge-like nanoribbons with low surface charge density but high aspect ratio remarkably enhance the membrane’s permeability and water stability, as verified by molecular simulations and experimental investigations. Using this approach, we developed a high-performance graphene oxide (GO) nanosheet/GO nanoribbon (GONR) nanofluidic membrane and achieved an ultrahigh power density of 18.1 W m–2 in a natural seawater|river water osmotic power generator, along with a high Coulombic efficiency and an extended lifespan in zinc metal batteries. The validity of our island-bridge structural design is also demonstrated for other nanosheet/nanoribbon composite membranes, providing a promising path for developing reliable aqueous energy conversion and storage devices.
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