Synergistic Effect of Hydrophilic Layers for Moisture‐Introduced Hybrid Power Generation

Hygroelectricity, converting chemical potential energy of abundant moisture from the atmosphere into electricity, is one of the most promising technologies in the development of next‐generation sustainable energy. Here, a uniquely designed hygroelectric generator is proposed with a stable self‐maintained water gradient and enhanced electricity generation by synergistic water transport in the multilayer structure, which boosts voltage and current outputs simultaneously as well as demonstrates a low environmental reliance. The devised multilayer structure facilitates charge separation of functional groups and boosts interfacial reactions with top electrodes, which first enabled a high voltage above 1.4 V in a wide range of humidity (0–85%) and an ultra‐high current of 1.15 mA (4.6 mA·cm −2 ) at 85% relative humidity due to hybrid energy contribution. The rechargeable moisture battery is achieved based on a hygroelectric generator and delivered a high Coulombic efficiency of 106%. The hygroelectric devices with high outputs are integrated into the self‐powered systems to charge a commercial mobile phone and achieve wearable human activity monitoring. Therefore, this work opens a bright prospect in achieving extremely high outputs with a low environmental reliance for sustainable energy generation systems.