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Sorption-based atmospheric water harvesting has the potential to realize water production anytime, anywhere, but reaching a hundred-gram high water yield in semi-arid climates is still challenging, although state-of-the-art sorbents have been used. Here, we report a portable and modularized water harvester with scalable, low-cost, and lightweight LiCl-based hygroscopic composite (Li-SHC) sorbents. Li-SHC achieves water uptake capacity of 1.18, 1.79, and 2.93 g g−1 at 15%, 30%, and 60% RH, respectively. Importantly, considering the large mismatch between water capture and release rates, a rationally designed batch processing mode is proposed to pursue maximum water yield in a single diurnal cycle. Together with the advanced thermal design, the water harvester shows an exceptional water yield of 311.69 g day−1 and 1.09 g gsorbent−1 day−1 in the semi-arid climate with the extremely low RH of ~15%, demonstrating the adaptability and possibility of achieving large-scale and reliable water production in real scenarios.

Sorption‐based atmospheric water harvesting (AWH) is a promising approach for mitigating worldwide water scarcity. However, reliable water supply driven by sustainable energy regardless of diurnal variation and weather remains a long‐standing challenge. To address this issue, a polyelectrolyte hydrogel sorbent with an optimal hybrid‐desorption multicyclic‐operation strategy is proposed, achieving all‐day AWH and a significant increase in daily water production. The polyelectrolyte hydrogel possesses a large interior osmotic pressure of 659 atm, which refreshes sorption sites by continuously migrating the sorbed water within its interior, and thus enhancing sorption kinetics. The charged polymeric chains coordinate with hygroscopic salt ions, anchoring the salts and preventing agglomeration and leakage, thereby enhancing cyclic stability. The hybrid desorption mode, which couples solar energy and simulated waste heat, introduces a uniform and adjustable sorbent temperature for achieving all‐day ultrafast water release. With rapid sorption–desorption kinetics, an optimization model suggests that eight moisture capture–release cycles are capable of achieving high water yield of 2410 mLwater kgsorbent−1 day−1, up to 3.5 times that of single‐cyclic non‐hybrid modes. The polyelectrolyte hydrogel sorbent and the coupling with sustainable energy driven desorption mode pave the way for the next‐generation AWH systems, significantly bringing freshwater on a multi‐kilogram scale closer.

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