Biomimetic Super‐Hygroscopic Metal–Organic Gel‐Based Moisture Pump for Humidity Regulation

Abstract Composites of “salt inside porous matrix” (CSPM) play a crucial role in indoor dehumidification and adsorption thermal management. However, the confined 3D structure of many host matrices typically limits the dispersion of salts and can lead to the leakage of hygroscopic salts, consequently reducing available sorption sites for water interaction. This restriction compromises both sorption capacity and kinetics, impeding the broader application of CSPM. In this work, a benign approach is proposed for fabricating 3D biomimetic metal–organic gels (MOGs). These MOGs feature an interconnected network that enables in situ encapsulation of low‐loading LiCl through a one‐pot process, achieving ≈100% yield. Benefiting from the moisture‐pump effect, the synthesized MOGs‐6LiCl exhibited a notable water vapor adsorption capacity of 1.07 g g −1 at 25 °C and 80% relative humidity, and maintained a long‐time stability with 0.98 g g −1 after 30 cycles. This exceptional performance stems from the uniform salt dispersion and minimum mass transfer hindrance in their gel network with hierarchical pores, surpassing the sum of adsorption capacities of its constituents linearly. Additionally, MOGs coatings demonstrate autonomous humidity regulation (±10% humidity difference) and thermal management capabilities under both laboratory and outdoor environments. These findings highlight their potential for integration into energy‐efficient adsorption‐based systems.