Chaotropic Effect‐Boosted Thermogalvanic Ionogel Thermocells for All‐Weather Power Generation

Abstract Ionic thermocells convert heat into electricity and are promising power sources for electronic devices. However, discontinuous and small electricity output limits practical use under varying environmental conditions. Here, a thermogalvanic ionogel with a high Seebeck coefficient (32.4 mV K⁻¹) is designed. Thermocells that combine thermogalvanic ionogel‐based thermocells, which realize all‐weather power generation via passive radiative cooling, are also developed. These thermocells generate electricity continuously under varying weather conditions and over a wide temperature range (−40 to 90 °C), with a normalized power density of 25.84 mW m⁻² K⁻². Advanced characterization shows that the chaotropic effect enhances the Seebeck coefficient, while the self‐supplying temperature difference given the radiative cooling structure enables all‐weather power generation. These results provide an effective strategy for developing practical thermocells suitable for diverse daily and seasonal variations.