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.
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