Developing ion‐selective membranes with anti‐biofouling property and biocompatibility is highly crucial in harvesting osmotic energy in natural environments and for future biomimetic applications. However, the exploration of membranes with these properties in osmotic energy conversion remain largely unaddressed. Herein, a tough zwitterionic gradient double‐network hydrogel membrane (ZGDHM) with excellent biofouling resistance and cytocompatibility for sustainable osmotic energy harvesting is demonstrated. The ZGDHM, composed of negatively charged 2‐acrylamido‐2‐methylpropanesulfonic acid (AMPS) as the first scaffold network and zwitterionic sulfobetaine acrylamide (SBAA) as the second network, is prepared by a two‐step photopolymerization, thus creating continuous gradient double‐network nanoarchitecture and then remarkably enhanced mechanical properties. As verified by the experiments and simulations, the gradient nanoarchitecture endows the hydrogel membrane with apparent ionic diode effect and space‐charge‐governed transport property, thus facilitating directional ion transport. Consequently, the ZGDHM can achieve a power density of 5.44 W m−2 by mixing artificial seawater and river water, surpassing the commercial benchmark. Most importantly, the output power can be promoted to an unprecedented value of 49.6 W m−2 at the mixing of salt‐lake water and river water, nearly doubling up most of the existing nanofluidic membranes. This study paves a new avenue toward developing ultrahigh‐performance osmotic energy harvesters for biomimetic applications.

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