Pyrrolic‐Nitrogen‐Enriched Aerogels With Magnetic Responsiveness Enable Cooperative Hydrogen‐Bond Regulation for High‐Performance Solar Interfacial Evaporation

ABSTRACT Although solar‐driven interfacial evaporation offers a sustainable pathway for desalination and wastewater remediation, its practical implementation remains limited by both the high vaporization enthalpy and rigid hydrogen‐bond network of water and performance degradation in complex water matrices. This study introduces a dual‐regulation strategy that integrates internal structural optimization with external‐field physical modulation. In particular, an Fe‐catalyzed pyrrole polymerization process yields a carbon‐based aerogel (CPP) with integrated ferromagnetism and enriched pyrrolic nitrogen sites. This synergy increases the intermediate‐water fraction, reduces vaporization enthalpy, and accelerates phase‐transition kinetics. Under one‐sun illumination (1 kW m ⁻² ), the CPP evaporator achieves an evaporation rate and efficiency of 2.78 kg m ⁻² h ⁻¹ and 84.0%, respectively, without magnetic assistance. After applying a 10 mT magnetic field, these values increase to 3.30 kg m ⁻² h ⁻¹ and 99.7%, respectively. Moreover, the system demonstrates stable salt self‐cleaning in seawater, resilience in organic wastewater, and multifunctionality in pollutant removal, achieving a tetracycline degradation rate of 89% when coupled with a solar‐driven advanced oxidation process. This study offers a generalizable framework that couples structural design with external‐field modulation for next‐generation solar evaporation systems.