High-strength shape-memory organohydrogel based on two orthogonal supramolecular effect: Gelator-induced phase-transition and metal-coordination interaction

• The organohydrogels can be synthesized by simple two-step procedures. • Our SN organohydrogels show high mechanical performances, comparable to DN gels. • The gelator endows liquid oil phase with switchable phase transition properties. • The orthogonal networks endow the gel with a dual-programming shape-memory property. • The shape-morphing behavior with high strength can be used for liquid transport. Shape-memory hydrogels are extensively applied in various fields. However, the existing shape-memory hydrogels with simple shape morphing, such as tensile and bending deformations, cannot satisfy complex and diverse requirements. When the hydrophilic and lipophilic structures were integrated into the same gel network, the heterogeneous structures can be separately controlled by two independent supramolecular interactions. Here, we prepared an organohydrogels with two orthogonal supramolecular networks (metal-coordination interaction of hydrogel framework and gelator-induced phase-transition of organogels inclusions) via photoinitiated polymerization and soaking in Fe 3+ solution. Importantly these two non-interfering orthogonal supramolecular networks endow the gel excellent mechanical properties and a unique dual-programmed shape-memory behavior, enabling highly accessible complex shape deformation, such as kirigami and multidimensional deformations. The organohydrogels can be used to fabricate smart devices for multidimensional on-demand fluid delivery. Consequently, our organohydrogel materials, with sophisticated and high-strength shape-memory properties, can further promote the practical application of gel materials in complex environments.