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Atmospheric water harvesting is urgently needed given increasing global waterscarcity. Current sorbent-based devices that cycle between water capture andrelease have low harvesting rates. We envision a radically differentmulti-material architecture with segregated and simultaneous capture andrelease. This way, proven fast-release mechanisms that approach theoreticallimits can be incorporated; however, no capture mechanism exists to supplyliquid adequately for release. Inspired by tree frogs and airplants, ourcapture approach transports water through a hydrogel membrane ``skin'' into aliquid desiccant. We report an extraordinarily high capture rate of 5.50$\text{kg}\,\text{m}^{-2}\,\text{d}^{-1}$ at a low humidity of 35%, limited bythe convection of air to the device. At higher humidities, we demonstrate up to16.9 $\text{kg}\,\text{m}^{-2}\,\text{d}^{-1}$, exceeding theoretical limitsfor release. Simulated performance of a hypothetical one-square-meter deviceshows that water could be supplied to two to three people in dry environments.This work is a significant step toward providing new resources to water-scarceregions.

High-yield atmospheric water capture via bioinspired material segregation