Macroscopic Layered Organogel–Hydrogel Hybrids with Controllable Wetting and Swelling Performance

Abstract 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.