to be faced. Therefore, it's necessary to develop a new nonliquid electrolyte with comprehensive performance for fulfilling various energy devices.Hydrogel electrolyte with hydrated salt crystal may be a new candidate to solve the above requirements by the introduction of new phase. The hydrated salt crystals, as one kind of industrial liquid-solid phase change materials, can be immobilized into hydrogel by the facile dissolution-crystallization transition. The demonstrated polymer gel electrolyte with NaAc·3H 2 O crystal as aligned porous template was designed by the in situ supersaturated crystallization of NaAc. [16,17] The introduction of inorganic crystal into polymer hydrogel can form the inorganic-organic composite with enhanced mechanical strength due to hydrogen bond or other synergistic effects. [18,19] The bound hydrated salt can suppress the electrochemical activity of water and broaden operating voltage of aqueous electrolyte [20] due to the strong interaction with water molecules, similar to the solvation sheath in "waterin-salt" electrolyte. [21][22][23] The high-concentrated salts within crystal-type gel can also efficiently reduce the freezing point and increase the boiling point of aqueous solutions. [24] At last, the hydrated salt crystal can endow gel electrolytes with thermalresistant performance through liquid-solid phase transition accompanied by endothermic and exothermic phenomena. [25,26] All in all, the crystal-type composite gel electrolyte can realize the comprehensive performance, including ultrahigh toughness, high operating voltage, extreme temperature tolerance, and good interfacial compatibility by a facile dissolution-crystallization transition approach.In this work, the pioneering crystal-type composite gel with excellent performance was prepared using a facile method that employed the crystallization of NaAc. There are only three main components in the precursor solution (Figure 1a,b): distilled water, abundant soluble salt, and a certain amount of monomer (or macromolecule). First, a high concentration of the salt solution was prepared by dissolving excessive soluble salt in the distilled water at high temperature. Then, the hydrogel was formed by UV irradiation for monomer solution (Figure 1c). Finally, the supersaturated salt within hydrogel was initiated to crystallize by placing a small crystal particle as seed on the surface of the hydrogel, and soon the crystal-type composite gel with extensive soluble salt crystals was obtained (Figure 1d). Typically, the crystal-type composite gel containing 15 wt% acrylamide (AAm) monomer and a certain quality of

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Octopus-inspired suckers, [6][7][8] fish-inspired adhesive disks, [9,10] tree-frog-inspired polygonal patterns, and [11,12] insect-inspired nanopillar arrays [13] achieve amazing wet adhesion performance by mimicking the peculiar micro/nanostructures of natural organisms. In addition, mussel-inspired innovative dopamine chemistry method has been actively employed to modify the surface with catecholamine functional groups. [14][15][16][17][18] Micro-nano etching and surface chemistry modification have become the mainstream of biomimetic adhesion design. Actually, climbing plants also exhibit ultrastrong adhesion for tightly bonding with the matrix. It is reported that creeper sucker can support a 22.9 t sperm whale within the palm-sized area (11.25 MPa). [19] Moreover, the adhesive discs were fully developed both for rough organic substrates like wood and smooth inorganic substrates like ceramic tiles. [20] Amazing adhesion and environmental adaptability have attracted scientists-eager attention to its adhesion mechanism.Actually, the creeper suckers adhere to supporting objects by flattening against the support surface and secreting the mucus at the base of the papillate cells. The mucus is highly heterogeneous, raftlike structure and consists of pectinaceous, rhamnogalacturonan (RG) I-reactive components surrounding a callosic core, which are subsequently lignified, and become hard by the deposition of polymers composed of phenylpropane derivative units. [21] In general, creeper utilizes the lignified polysaccharide mucilage in the sucker to adhere to hard/soft interface simultaneously in harsh climate. Accordingly, the optimized curable organic matter that can noncovalently reinforce polymer network should be a feasible strategy to manufacture the creeper sucker-inspired adhesive materials.Crystalline ionic liquid is a kind of salt whose phase-transition is fully controllable due to its own low melting point. Similar to the raft-shaped lignified polysaccharide, the crystalline ionic liquid presents dendritic fibers, [22] which becomes a promising filler to simulate the adhesion behavior of creeper sucker.Herein, we develop a simple and robust strategy to design polymer gel adhesive inspired by creeper sucker. Crystallizable 1-ethyl-3-methylimidazolium bromide ([EMIM]Br) solvent High-strength and reversible adhesion technology, which is a universal phenomenon in nature but remains challenging for artificial synthesis, is essential for the development of modern science. Existing adhesive designs without interface versatility hinder their application to arbitrary surfaces. Bioinspired by creeper suckers, a crystal-fiber reinforced polymer gel adhesive with ultrastrong adhesion strength and universal interface adaptability is creatively prepared via introducing a room-temperature crystallizable solvent into the polymer network. The gel adhesive formed by hydrogen bonding interaction between crystal fibers and polymer network can successfully realize over 9.82 MPa reversible adhesion strength for rough interface and...

Bioelectronic platforms convert biological signals into electrical signals by utilizing biocatalysts that provide tools to monitor the activity of cells and tissues. Traditional conducting materials such as solid conductors and conducting polymers are confronted with a great challenge in sophisticated production processes and mismatch at biological tissues–machine interfaces. Furthermore, the biocatalyst, the key functional component in the electron‐transfer reaction for bio‐signal detection denatures easily in an ionic conductive solution. Herein, a bionic strategy is elaborately developed to synthesize an ionohydrogel bioelectronic platform that possesses extracellular‐matrix‐like habitat by employing hydrated ionic liquids (HILs) as ionic solvent and bioprotectant. This strategy realizes an integration of ionic and enzymatic electronic circuits and minimization of the disparities between tissues and artificial machines. The Hofmeister effect of HILs on enzyme proteins and polymer chains ensures the high bioactivity of the enzymes and greatly improves the mechanical properties of the ionohydrogels. Moreover, hydrogen bonds formed by ILs, water, and polymer chains greatly improve the water‐retention of the ionohydrogel and give it more practical significance. Consequently, the promising ionohydrogel is partly printed and fabricated into wearable devices as a pain‐free humoral components monitor and a wireless motion‐sensor.