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Safe and adequate water is a global challenge due to the growing population and environmental pollution. Access to clean water is a cornerstone for the further development of our society. Thermal and membrane-based technologies have been developed to increase water supplies via seawater desalination and sewage recycling. However, the requirement of considerable energy consumption and frequent maintenance of infrastructures have raised a barrier for economically stressed and off-grid communities. In this talk, I will present how to design hydrogel materials, from molecular-level building blocks to microscopic structures and surface properties, for efficient solar-powered desalination and water purification. First, the hydrophilic polymeric mesh of hydrogels interacts with water in a unique way that energy demand for water evaporation can be lowered; hence, water can evaporate much faster from hydrated hydrogels. Next, surface wettability, topography, and overall structures can be controlled by polymer chemistry-guided synthesis and processing, leading to substantial improvement in the clean water yield. Moreover, by material selection and molecular engineering, heavy metal-ion adsorption, antibacterial, and anti-biofouling features can be incorporated for rapid water purification without additional energy input. Last, what if the communities are far from the ocean or water bodies? I will discuss the design of hygroscopic polymer films to harvest water from arid air, regardless of geographical or hydrologic conditions. With simple, scalable fabrication and cost-effectiveness, hydrogels are emerging as a promising material platform for applications in the sustainable water-energy-environmental nexus.