Customized Microenvironments Spontaneously Facilitate Coupled Engineering of Real‐Life Large‐Scale Clean Water Capture and Pollution Remediation

Abstract Harnessing abundant renewable resources and pollutants on a large scale to address environmental challenges, while providing sustainable freshwater, is a significant endeavour. This study presents the design of fully functional solar vaporization devices (SVD) based on organic–inorganic hybrid nanocomposites (CCMs‐x). These devices exhibit efficient photothermal properties that facilitate multitargeted interfacial reactions, enabling simultaneous catalysis of sewage and desalination. The localized interfacial heating generated by the photothermal effect of CCMs‐x triggers surface‐dominated catalysis and steam generation. The CCMs‐x SVD achieves a solar water‐vapor generation rate of 1.41 kg m⁻² h⁻¹ (90.8%), and it achieves over 95% removal of pollutants within 60 min under one‐sun for practical application. The exceptional photothermal conversion rate of wastewater for environmental remediation and water capture is attributed to customized microenvironments within the system. The integrated parallel reaction system in SVD ensures it is a real‐life application in multiple scenarios such as municipal/medical wastewater and brine containing high concentrations. Additionally, the SVD exhibits long‐term durability, antifouling functionality toward complex ionic contaminants. This study not only demonstrates a one‐stone–two‐birds strategy for large‐scale direct production of potable water from polluted seawater, but also opens up exciting possibilities for parallel production of energy and water resources.