Many biological organisms can tune their mechanical properties to adapt to environments in multistable modes, but the current synthetic materials, with bistable states, have a limited ability to alter mechanical stiffness. Here, we constructed programmable organohydrogels with multistable mechanical states by an on-demand modular assembly of noneutectic phase transition components inside microrganogel inclusions. The resultant multiphase organohydrogel exhibits precisely controllable thermo-induced stepwise switching (i.e., triple, quadruple, and quintuple switching) mechanics and a self-healing property. The organohydrogel was introduced into the design of soft-matter machines, yielding a soft gripper with adaptive grasping through stiffness matching with various objects under pneumatic-thermal hybrid actuation. Meanwhile, a programmable adhesion of octopus-inspired robotic tentacles on a wide range of surface morphologies was realized. These results demonstrated the applicability of these organohydrogels in lifelike soft robotics in unconstructed and human body environments.

A fabrication strategy for biphasic gels is reported, which incorporates high-internal-phase emulsions. Closely packed micro-inclusions within the elastic hydrogel matrix greatly improve the mechanical properties of the materials. The materials exhibit excellent switchable mechanics and shape-memory performance because of the switchable micro- inclusions that are incorporated into the hydrogel matrix. The produced materials demonstrated a self-healing capacity that originates from the noncovalent effect of the biphasic heteronetwork. The aforementioned characteristics suggest that the biphasic gels may serve as ideal composite gel materials with validity in a variety of applications, such as soft actuators, flexible devices, and biological materials.

for applications in aerospace, smart devices, and biomedical materials. [1][2][3] Among these materials, shape-morphing polymers (SMPs) are particularly attractive because their forms can be programmed to perform transformations or motions in response to external stimuli (e.g., temperature, light, solvent, and electric fields). [3][4][5][6][7][8][9][10][11] Currently, two general approaches are used to obtain unparalleled shape-programming flexibility. The first involves geometric assistances to produce complex SMP shapes, such as kirigami and origami art, as well as 3D printing. [12][13][14][15][16][17] Alternatively, another approach is through the use of an innovational polymer network design, which employs functional components to expand the programmability of SMPs. [18][19][20][21][22][23] For example, SMPs with dynamic covalent polymer networks and reversible crosslinking netpoints exhibit unique shape reconfiguration and programmability. [18][19][20][21] However, despite these exciting prospects, most SMPs with the single control routes only allow complex temporary shapes to recover a former permanent state, ultimately limiting the versatility of these materials and our ability to control them for complex applications. Owing to the intrinsic restriction of the permanently crosslinked polymer network, such single programming inevitably lacks a mechanism Programmable materials that can change their inherent shapes or properties are highly desirable due to their promising applications. However, among various programmable shape-morphing materials, the single control route allows temporary states to recover the unchangeable former state, thus lacking the sophisticated programmability for their shape-encoding behaviors and mechanics. Herein, dual-programmable shape-morphing organohydrogels featuring supramolecular heteronetworks are developed. In the system, the metallo-supramolecular hydrogel framework and micro-organogels featuring semicrystalline comb-type networks independently respond to different stimuli, thereby providing orthogonal dual-switching mechanics and ultrahigh mechanical strength. The supramolecular heteronetworks also possess excellent self-healing properties. More notably, such orthogonal supramolecular heteronetworks demonstrate hierarchical shape morphing performance that far exceeds conventional shape-morphing materials. Utilizing this dual programming strategy of the orthogonal supramolecular heteronetworks, the material's permanent shape can be manipulated in a step-wise shape morphing process, thereby realizing sophisticated shape changes with a high degree of freedom. The organohydrogels can act as a biomimetic smart device for the on-demand control of unidirectional liquid transport. Based on these characteristics, it is anticipated that the supramolecular organohydrogels may serve as adaptive programmable materials for a variety of applications. Gel MaterialsProgrammable materials are capable of changing their inherent shapes or exquisite properties to adapt to complex environments a...

Adaptive materials with reconfigurable surface topography in response to external environments have attracted considerable attention in various fields. Here, adaptive superamphiphilic organohydrogels with reconfigurable surface topography are reported, featuring a high degree of freedom. The organohydrogels can simultaneously adapt to different surrounding mediums and reversibly switch between hydrogel-and organogeldominated surface reconfigurations to realize adaptive superhydrophilic and superoleophilic transitions. Meanwhile, these adaptive organohydrogels possess a heteronetwork complementary effect to elicit surface self-healing capacity. Importantly, owing to these organohydrogels' reversible wettability transition, excellent surface morphing performance and bioinspired strategy, various geometrically complex biomimetic topographies can be programmed, offering unique unidirectional transport for opposite-featured liquids in multimedia environments. Smart organohydrogel-based microfluidic devices are also developed for on-demand remote programming of liquid transport. Therefore, the organohydrogels suggest a reconfigurable surface topography design strategy, and would act as adaptive programmable materials for smart surface applications.

Flexible pressure sensors usually require functional materials with both mechanical compliance and appropriate electrical performance. Most sensors based on materials with limited compressibility can hardly balance between high sensitivity and broad pressure range. Here, we prepare a heterophasic ionogel with shape and stiffness memory for adaptive pressure sensors. By combining the microstructure alignment for stiffness changing and shape memory micro-inclusions for stiffness fixing, the heterophasic ionogels reveal tunable compressibility. This controllable pressure-deformation property of the ionogels results in the pressure sensors’ programmable pressure-resistance behavior with tunable pressure ranges, varied detection limits, and good resolution at high pressure. Broad pressure ranges to 220 and 380 kPa, and tunable detection limit from 120 to 330 and 950 Pa are realized by the stiffness memory ionogel sensors. Adaptive detection is also brought out to monitor tiny pressure changes at low stiffness and distinguish different human motions at high stiffness. Using shape and stiffness memory materials in pressure sensors is a general design to achieve programmable performance for more complex application scenarios.