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  1. Free, publicly-accessible full text available December 30, 2023
  2. Multi-functional membranes with high permeance and selectivity that can mimic nature's designs have tremendous industrial and bio-medical applications. Here, we report a novel concept of a 3D nanometer (nm)-thin membrane that can overcome the shortcomings of conventional membrane structures. Our 3D membrane is composed of two three-dimensionally interwoven channels that are separated by a continuous nm-thin amorphous TiO 2 layer. This 3D architecture dramatically increases the surface area by 6000 times, coupled with an ultra-short diffusion distance through the 2 – 4 nm-thin selective layer that allows for ultrafast gas and water transport, ∼900 l m −2 h −1 bar −1 . The 3D membrane also exhibits a very high ion rejection ( R ∼ 100% for potassium ferricyanide) due to the combined size- and charge-based exclusion mechanisms. The combination of high ion rejection and ultrafast permeation makes our 3DM superior to the state-of-the-art high-flux membranes whose performances are limited by the flux-rejection tradeoff. Furthermore, its ultimate Li + selectivity over polysulfide or gas can potentially solve major technical challenges in energy storage applications, such as lithium – sulfur or lithium – O 2 batteries.