High Performance Moisture‐Electricity Generator Aerogel With Ultrahigh/Gradual Ion Concentration Gradient, Wettability Gradient and Oriented Porous Structure

ABSTRACT Moisture‐electricity generators (MEGs), which directly convert environmental humidity into electricity, remain limited by low power output, short operational lifetimes, and insufficient cycling stability. We introduce an oriented aerogel‐based MEG with ultrahigh/gradual ion concentration gradient and wettability gradient architecture. Fabricated via turbulent shear precipitation, semi‑layer‑by‑layer gelation, and directional freezing, the MEG features three trilayered layers where modulated filler content establishes a gradual ion‑concentration gradient, thereby enabling sustained charge‑carrier propulsion. Non‐covalent functionalization of single‐walled carbon nanotubes (SWNTs) with ionic liquids and surfactants enhances dispersion and establishes a substantial ion‐concentration gradient (−38 mV to +38.8 mV), while turbulent‐shear precipitation produces a dendritic polymer framework that intertwines with the SWNTs into a core–shell architecture, thereby enlarging the SWNT–water interfacial area. A tunable wettability gradient (water contact angle: 31.31°–111.21°) ensures sustained water and charge transport. Fabrication via semi‐layer‐by‐layer gelation self‐assembly prevents interlayer separation and excessive mixing. Directional freezing yields aligned porous structures that shorten transport pathways while reinforcing mechanical durability. Leveraging multi‐gradient synergy and process optimization, the device delivers record‐breaking overall performances: an energy density of 826.15 µW·h·cm − 2 and power density of 162.95 µW·cm − 2 , stable operation over 100 h, maintains over 85% of its capacity after 10 cycles, and maintains performance after one‑month storage.