Soft gels that integrate the water retention of hydrogels and the water swelling resistance of organogels are sought by researchers. Such materials have useful properties and potential applications in stretchable and biointegrated fields, such as tissue engineering, microfluidics, and biomedical devices. This study reports a simple yet versatile method for assembling hydrogels and organogels into covalently tethered hybrids to provide robust properties, such as excellent stretchability, tough interfacial bonds, enduring antiswelling, and low dehydration. The proposed method is simple and can generally be applied to hydrogels that contain hydroxyl terminal groups and commonly used organogels that can copolymerize with double‐bond groups. The unique property of being externally hydrophobic and internally hydrophilic enables the organogel–hydrogel hybrids to be applied to many fields, such as mobility control of water droplets, printing, and 3D structure development. The organogel hydrogel hybrids not only present superior wettability performances, such as water retention and swelling resistance, but also present applicable functions that make them useful in tissue engineering and biomedical devices in vivo.

Solar-driven water evaporation is considered to be an appealing way to solve water scarcity issues globally. Various natural creatures possess unique structural features and exhibit an excellent pumping ability in arid environments. Motivated by sunflower stalk pith, here, the biomass porous foam modified with zwitterionic hydrogel coating for solar desalination devices is introduced. It is demonstrated that the multi-curvature and gradient honeycomb architecture offers a remarkable solar desalination system, which combines critical aspects of solar evaporation including high light absorption, localizing converted heat, rapid water transport, water activation, and multi-channel release of steam via its ubiquitous structure, and substantially outperforms other natural biomass materials. The device exhibits long-term stability in actual seawater, as well as high performance for soybean oil emulsion and oily brines (crude oil, salts). Furthermore, the long-term use of excellent storability to prevent putrefying is shown, which is attributed to the outstanding antifouling property of zwitterionic hydrogel. It is envisioned that the nature material with the advantage of being inexpensive, environmentally friendly, and portable, may be a new candidate for water purification and desalination.