Ionic Crosslinking Research Articles

Effect of halloysite nanotubes on the self-healing performance of natural rubber nanocomposites enabled by reversible zinc thiolate networks

This article presents the high loading halloysite nanotubes, Hals (20, 30, 40 and 50 phr) filled self-healing natural rubber nanocomposites crosslinked via ionic bonding networks. The reinforcing effect of high loading Hals on self-healing recovery and mechanical performance of NR were thoroughly examined and characterized by TEM, FT-IR, TGA, SEM, DMA, Anton Paar rheometer, and compression set analysis. It was observed that the high Hals content resulted in 100% improvement in tensile strength with an excellent healing recovery of up to 85% at room temperature without any external source. The reversible network structure formed via ionic crosslinks and its stability was identified by FTIR. TGA results revealed that the developed nanocomposites showed enhanced thermal stability compared to unfilled NR. Scanning Electron Microscopy (SEM) micrographs showed that the healed interfaces adhered well when the cut pieces were merged, suggesting that intermolecular diffusion occurred at the fractured surfaces. Overall, this study provides valuable insights into the reinforcing effects of Hals at higher loading on the structure and performance of self-healing natural rubber.

Soybean protein isolate-sodium alginate double network emulsion gels: Mechanism of formation and improved freeze-thaw stability

Soybean protein isolate (SPI) is widely used in the food industry. However, SPI-based emulsion gels tend to aggregate and undergo oiling-off during freeze-thawing. In this study, emulsion gels were prepared by a combination of heat treatment and ionic cross-linking using SPI and sodium alginate (SA) as raw materials. The focus was on exploring the mechanistic effects of the SPI-SA double network structure on the freeze-thaw stability of emulsion gels. The results showed that the addition of SA could form different types of network structures with SPI, due to different degrees of phase separation. In addition, SA appearing on the SPI network indicated that the addition of Ca2+ shielded the electrostatic repulsion between SPI and SA to form SPI-SA complexes. The disappearance of the characteristic peaks of SA and SPI in Fourier transform infrared spectroscopy analysis also confirmed this view. Low-field nuclear magnetic resonance data revealed that SA played a role in restricting water migration within the emulsion gels, increasing bound water content, and thereby improving the water-holding capacity of the emulsion gels. Therefore, the incorporation of SA improved the freeze-thaw stability of SPI emulsion gels. These findings offer a theoretical basis and technical support for SPI application in frozen products.

Impact of calcium-starch interactions on the textural and oil absorption properties of deep-fried potato mashes

The quality of mashed potato-based deep-fried products largely depends on their texture and oil content. In this study, Laser Ablation Inductively Coupled Plasma Mass Spectrometry analysis revealed that CaCl2 addition to the water used for blanching increased the presence of Ca2+ ions in potato cell walls, in the middle lamellae as well as in the cells. Potato mashes were softer and had lower storage and loss moduli when the CaCl2 concentration was increased. Similar observations were made for potato starch gels, highlighting the importance of the interactions between Ca2+ ions and starch for the properties of potato mashes. Interestingly, more amylose was extracted from potato starch gels when the system contained more CaCl2 due to increased amylose leaching from the granules and impaired crystallization. In contrast, amylopectin extraction yields were hardly affected. It is suggested that in potato mashes, the presence of more extracellular amylose with lower crystallinity changed the textural and rheological properties when CaCl2 was added to the blanching water. Additionally, Time Domain Proton Nuclear Magnetic Resonance revealed more and stronger interactions between starch and water in potato mashes due to Ca2+ ions cross-linking amylopectin. These stronger interactions are believed to contribute to the observed reduced oil absorption during deep-frying. Hence, CaCl2 addition during blanching can impact the quality of deep-fried potato mashes and holds promise to optimize the manufacture of frozen potato products.

Glassy gels toughened by solvent.

Glassy polymers are generally stiff and strong yet have limited extensibility1. By swelling with solvent, glassy polymers can become gels that are soft and weak yet have enhanced extensibility1-3. The marked changes in properties arise from the solvent increasing free volume between chains while weakening polymer-polymer interactions. Here we show that solvating polar polymers with ionic liquids (that is, ionogels4,5) at appropriate concentrations can produce a unique class of materials called glassy gels with desirable properties ofboth glasses and gels. The ionic liquid increases free volume and therefore extensibility despite the absence of conventional solvent (for example, water). Yet, the ionic liquid forms strong and abundant non-covalent crosslinks between polymer chains to render a stiff, tough, glassy, and homogeneous network (that is, no phase separation)6, at room temperature. Despite being more than 54 wt% liquid, the glassy gels exhibit enormous fracture strength (42 MPa), toughness (110 MJ m-3), yield strength (73 MPa) and Young's modulus (1 GPa). These values are similar to those of thermoplastics such as polyethylene, yet unlike thermoplastics, the glassy gels can be deformed up to 670% strain with full and rapid recovery on heating. These transparent materials form by a one-step polymerization and have impressive adhesive, self-healing and shape-memory properties.

Preparation and Characterization of Silica-Coated Sodium Alginate Hydrogel Beads and the Delivery of Curcumin

In this study, to address the defects of sodium alginate (SA), such as its susceptibility to disintegration, silica was coated on the outer layer of sodium alginate hydrogel beads in order to improve its swelling and slow-release properties. Tetraethyl orthosilicate (TEOS) was used as the hydrolyzed precursor, and the solution of silica precursor was prepared by sol-gel reaction under acidic conditions. Then SA–silica hydrogel beads prepared by ionic crosslinking method were immersed into the SiO2 precursor solution to prepare SA–silica hydrogel beads. The chemical structure and morphology of the hydrogel beads were characterized by XRD, FTIR, and SEM, and the results showed that the surface of SA–silica beads was successfully encapsulated with the outer layer of SiO2, and the surface was smooth and dense. The swelling experiments showed that the swelling performance effectively decreased with the increase of TEOS molar concentration, and the maximum swelling ratio of the hydrogel beads decreased from 41.07 to 14.3, and the time to reach the maximum swelling ratio was prolonged from 4 h to 8 h. The sustained-release experiments showed that the SA–silica hydrogel beads possessed a good pH sensitivity, and the time of sustained-release was significantly prolonged in vitro. Hemolysis and cytotoxicity experiments showed that the SA-silica hydrogel beads were biocompatible when the TEOS molar concentration was lower than 0.375 M. The SA–silica-2 hydrogel beads had good biocompatibility, swelling properties, and slow-release properties at the same time.

Colorimetric sensor to monitor the temperature with in situ synthesized silver nanoparticles embedded in carboxymethyl cellulose metallogel

A colorimetric sensing platform based on carboxymethyl cellulose-silver nanoparticles (CMC-AgNPs) metallogel was proposed to monitor the temperature history and quality of perishable products stored at low temperature. The carboxymethyl cellulose (CMC) metallogel, fabricated in the presence of Ag+, incorporates ionic crosslinking of biopolymers, complexation between reactants, and subsequent in situ synthesis of AgNPs, which are designed to lead the color transition of metallogel from colorless to dark brown depending on temperature and time. The mechanical and structural properties of metallogels and AgNPs were characterized by rheology, XRD, and FT-IR. Color changes associated with temperature, time, and metal ion precursors were examined by UV–visible spectroscopy and colorimetry. The longer the exposure time to thermal stress condition such as room temperature (25 °C) or high temperature (60 °C), the deeper the color of metallogel. The CMC-AgNPs metallogel-based sensor provides an efficient, safe way to track temperature history and assess perishable products’ quality, crucial for the safe distribution of food, vaccines, and medicines. This cost-effective and reliable visual sensor minimizes spoilage and health risks by enabling accurate temperature monitoring without the need for complicated equipment.

Construction of Tough Hydrogel Cross-Linked via Ionic Interaction by Protection Effect of Hydrophobic Domains.

Most hydrogels have poor mechanical properties, severely limiting their potential applications, and numerous approaches have been introduced to fabricate more robust and durable examples. However, these systems consist of nonbiodegradable polymers which limit their application in tissue engineering. Herein, we focus on the fabrication and investigate the influence of hydrophobic segments on ionic cross-linking properties for the construction of a tough, biodegradable hydrogel. A biodegradable, poly(γ-glutamic acid) polymer conjugated with a hydrophobic amino acid, l-phenylalanine ethyl ester (Phe), together with an ionic cross-linking group, alendronic acid (Aln) resulting in γ-PGA-Aln-Phe, was initially synthesized. Rheological assessments through time sweep oscillation testing revealed that the presence of hydrophobic domains accelerated gelation. Comparing gels with and without hydrophobic domains, the compressive strength of γ-PGA-Aln-Phe was found to be six times higher and exhibited longer stability properties in ethylenediaminetetraacetic acid solution, lasting for up to a month. Significantly, the contribution of the hydrophobic domains to the mechanical strength and stability of ionic cross-linking properties of the gel was found to be the dominant factor for the fabrication of a tough hydrogel. As a result, this study provides a new strategy for mechanical enhancement and preserves ionic cross-linked sites by the addition of hydrophobic domains. The development of tough, biodegradable hydrogels reported herein will open up new possibilities for applications in the field of biomaterials.

Stepwise reinforcement strategy for guar gum/sodium alginate based films: Introduction of carboxylated cellulose nanofibers by different methods and further calcium ion crosslinking

Insufficient mechanical, barrier and water resistance properties of guar gum (GG) films limit their application in food packaging field. Herein, the properties of GG films were enhanced by a stepwise modification strategy. The mechanical and water vapor barrier properties of GG films were initially reinforced by doping with a different type of polysaccharide (sodium alginate; SA). Next, carboxylated cellulose nanofibers (CCN) were introduced as a reinforcing agent to improve film properties via two methods (blending and layer-by-layer (LBL) assembly method). Finally, the water resistance of composite films was further enhanced by calcium ion cross-linking treatment. GG/SA composite films exhibited better mechanical strength and water vapor barrier capacity compared to pristine GG film. In addition, the introduction of CCN, either by blending or LBL method, improved the light barrier, water vapor barrier and tensile strength. The calcium ion cross-linking treatment further enhanced the water vapor barrier, thermal stability, tensile strength and water resistance capacity. The potential applications of GG/SA/CCN films in real food packaging were also explored. In short, this study presents a simple and feasible performance enhancement strategy for GG and other underperforming polysaccharide matrix films, with potential applications in the development of high-performance bio-based food packaging materials.

Effects of Mineral Elements and Annealing on the Physicochemical Properties of Native Potato Starch

Native potato starch is an excellent carrier of minerals due to its inherent ion exchange capacity. Mineral enrichment not only changes the nutritional value but also influences starch pasting and swelling properties. Hydrothermal treatments like annealing constitute a straightforward and green way to tune functional properties. Here, novel combinations of mineral enrichment and annealing were studied. Ion exchange was readily achieved by suspending starch in a salt solution at room temperature over 3 h and confirmed by ICP-OES. Annealing at 50 °C for 24 h using demineralized water or salt solutions strongly affected pasting, thermal, and swelling properties. The obtained XRD and DSC results support a more ordered structure with relative crystallinity increasing from initially 41.7% to 44.4% and gelatinization onset temperature increasing from 60.39 to 65.94 J/g. Solid-state NMR spectroscopy revealed no detectable changes after annealing. Total digestible starch content decreased after annealing from 8.89 to 7.86 g/100 g. During both ion exchange at room temperature and annealing, monovalent cations promoted swelling and peak viscosity, and divalent cations suppressed peak viscosity through ionic crosslinking. The presented combination allows fine-tuning of pasting behavior, potentially enabling requirements of respective food applications to be met while offering an alternative to chemically modified starches.

Self-Evolving Hierarchical Hydrogel Fibers with Circadian Rhythms and Memory Functions.

The fusion of hierarchical tissues at interfaces, incorporating ultrafast selective transport channels, enables efficient matter exchange and energy transfer across multiscale structures in living organisms. However, achieving these characteristics simultaneously in an artificial multimaterial system is challenging. Here, this work presents a multimaterial hydrogel fiber with a hierarchical structure of interface fusion, which forms spontaneously through in situ hierarchy evolution induced by ionic cross-linking and molecular shear flow. Water transport occurs in the angstrom-scale confined slits created by aligned cellulose nanocrystals (CNCs) by direct Coulomb knock-on, resembling Newton's cradle motion. The fusion of interfaces enables high-efficiency water transport across multiscale layers, combined with Newton's cradle-like collective water motion, creating a highly sensitive negative feedback loop within the fiber. These fibers exhibit integrated behaviors of time-space perception, short-term memory and adaptive changes in shape. Additionally, they demonstrate rhythm characteristics, changing periodically in a 24-h day-night cycle. Composed of natural building blocks, these hierarchical hydrogel fibers exhibit a memristor effect similar to that of an elementary neuron, making them promising for applications in seamless on-skin and implantable bioelectronics.

Preparation of Cross-Linked Sodium Alginate Microspheres with Different Metal Ions Using the Microfluidic Electrospray Technology.

Microspheres are micrometer-sized particles that can load and gradually release drugs via physical encapsulation or adsorption onto the surface and within polymers. In the field of biomedicine, hydrogel microspheres have been extensively studied for their application as drug carriers owing to their ability to reduce the frequency of drug administration, minimize side effects, and improve patient compliance. Sodium alginate (ALG) is a naturally occurring linear polysaccharide with three backbone glycosidic linkages. There are two auxiliary hydroxyl groups present in each of the moieties of the polymer, which have the characteristics of an alcohol hydroxyl moiety. The synthetic ALG units can undergo chemical cross-linking reactions with metal ions, forming a cross-linked network structure of polymer stacks, ultimately forming a hydrogel. Hydrogel microspheres can be prepared using a simple process involving the ionic cross-linking properties of ALG. In this study, we prepared ALG-based hydrogel microspheres (ALGMS) using a microfluidic electrodeposition strategy. The prepared hydrogel microspheres were uniformly sized and well-dispersed, owing to accurate control of the microfluidic electrospray flow. ALGMS cross-linked with different metal ions were prepared using a microfluidic electrospray technique combining microfluidic and high electric field, and its antimicrobial properties, slow drug release ability, and biocompatibility were investigated. This technology holds promise for application in advanced drug development and production.

Physicochemical, structural, and in-vitro release properties of carboxymethyl cellulose-based cryogel beads incorporating resveratrol-loaded microparticles for colon-targeted delivery system

The objective of this study was to investigate the physicochemical, structural, and in vitro release properties of carboxymethyl cellulose (CMC)-based cryogel beads incorporating resveratrol-loaded microparticles (MP) for colon-targeted delivery system. CMC-based cryogel beads were produced by ionic cross-linking with different concentrations (2%, 3%, and 4%) of AlCl3. Based on FE-SEM images, CMC-based cryogel beads showed a smoother surface and more compact internal structure with increasing AlCl3 concentrations, which was proven to be due to the new cross-linking between the –COO− group of CMC and Al3+ by FT-IR analysis. The encapsulation efficiency of the cryogel beads was significantly increased from 79.48% to 85.74% by elevating the concentrations of AlCl3 from 2% to 4%, respectively. In vitro release study showed that all CMC-based cryogel beads had higher stability for resveratrol than MP in simulated gastric conditions and can efficiently deliver resveratrol to colon without the premature release.

Bio-Inspired Screwed Conduits from the Microfluidic Rope-Coiling Effect for Microvessels and Bronchioles

Tubular microfibers have recently attracted extensive interest for applications in tissue engineering. However, the fabrication of tubular fibers with intricate hierarchical structures remains a major challenge. Here, we present a novel one-step microfluidic spinning method to generate bio-inspired screwed conduits (BSCs). Based on the microfluidic rope-coiling effect, a viscous hydrogel precursor is first curved into a helix stream in the channel, and then consecutively packed as a hollow structured stream and gelated into a screwed conduit (SC) via ionic and covalent crosslinking. By taking advantage of the excellent fluid-controlling ability of microfluidics, various tubes with diverse structures are fabricated via simple control over fluid velocities and multiple microfluidic device designs. The perfusability and permeability results, as well as the encapsulation and culture of human umbilical vein endothelial cells (HUVECs), human pulmonary alveolar epithelial cells (HPAs), and myogenic cells (C2C12), demonstrate that these SCs have good perfusability and permeability and the ability to induce the formation of functional biostructures. These features support the uniqueness and potential applications of these BSCs as biomimetic blood vessels and bronchiole tissues in combination with tissue microstructures, with likely application possibilities in biomedical engineering.

A universal solvent-replacement strategy to convert alginate hydrogels into mechanically strong and transparent alginate eutectogels for sensitive strain sensors

Eutectogels based on natural polymers have attracted significant attention as an alternative to easily dehydrated hydrogels and expensive ionogels in the development of flexible strain sensors. The feasibility of employing eutectogels derived from pure natural polymers could be greatly enhanced if their mechanical properties satisfy the requirements of applications. Herein, alginate eutectogels (AEs) with high mechanical properties (tensile strain 217 % and strength 2.26 MPa at fracture), and excellent transparency (over 90 %) are acquired via CaCl2 inducing ionic crosslinking and subsequent deep eutectic solvents (DESs, composed of glycerol and choline chloride) initiating physical crosslinking with a universal solvent- replacement strategy. Among them, sodium alginate, a natural polysaccharide polymer, is selected as representative supporting scaffolds and forms water-insoluble alginate hydrogels (AHs) in CaCl2 coagulation bath. The exchange of DESs with water of AHs not only restrengthens the polymer network by physical crosslinking, but also endows the obtained AEs with long-term solvent retention and high temperature resistance. In addition, the AEs not only have high reliability but also exhibit better linear sensitivity in a wide strain range (0–200 %). In particular, the AEs display multiple sensitivity to stretching, bending, and human motions, demonstrating feasibility as sensitive strain sensors.

Rheological study of hybrid aqueous suspension of TEMPO-oxidized cellulose nanofibrils and graphene oxide

The incorporation of graphene oxide (GO) into a nanocellulose matrix has attracted considerable attention due to the unique advantages of both components. This study focuses on investigating the viscoelastic and flow properties of hybrid aqueous suspensions (2.00 w/v%), composed of TEMPO-oxidized cellulose nanofibrils (TOCNF) and GO at different TOCNF/GO weight ratios. To adjust the elastic properties of the hybrid suspensions, calcium ions are introduced, varying the concentration systematically to study their effects on the hybrid network structure. All blends exhibit shear-thinning behaviour and demonstrate elastic, gel-like properties. Notably, in the absence of calcium ions, the enhancement of elastic properties is more pronounced at higher GO fractions. Conversely, with the introduction of calcium ions, the enhancement of elastic properties becomes particularly important at higher TOCNF fractions. For the quantitative evaluation of these enhancements, we employ the logarithmic mixing rule. Significant positive deviations from the predictions of the logarithmic mixing rule are ascribed to the complex, concentration-dependent arrangement of cellulose nanofibrils and GO liquid crystals in the aqueous suspension, coupled with ionic crosslinking induced by calcium ions. The study aims to contribute to the understanding of the rheological behaviour of the TOCNF/GO hydrogel, showing potential advancements in various applications.Graphical abstract

Efficient zinc protection enabled by polyhedral metal-organic framework and ionic-crosslinking binder

Towards the efficient reversibility and cyclability of Zinc (Zn) plating/stripping, surface modification has been recognized as one of the straightforward strategies for Zn electrodes. In this study, 20 μm of a composite layer prepared by blending ZIF-8 and sodium alginate (SA) was uniformly coated on the Zn foil (Z8-SA@Zn) as an alternative protective layer to explore their synergistic contributions in suppressing the side reaction under the aqueous electrolyte. Benefiting from the following characteristics: (a) ionic crosslinking between SA and Zn2+, (b) improved Zn2+ flux, (c) more hydrophilic / zincophilic, and (d) chemical stability, the resulting Z8-SA@Zn revealed the remarkably anti-corrosive property, insignificant zincate growth, high Coulombic efficiency, and prolong cyclability. Encouragingly, the zinc-ion hybrid supercapacitor assembled by Z8-SA@Zn anode and commercial activated carbon cathode not only delivers an impressive rate capability (45 mAh/g at 1 mA/cm2, 37 mAh/g at 10 mA/cm2) but also achieves the excellent cycling stability (capacity retention: 91 % after 20,000 cycles at 5 mA). According to the results disclosed here, combining ZIF-8 and SA as the interfacial layer provides multifunctional features, enabling the effective protection of Zn foil. Consequently, it is rationally believed that the Z8-SA@Zn can be a promising anode material for Zn2+ storage applications.

Preparation of a Flame-Retardant Curing Agent Based on Phytic Acid-Melamine Ion Crosslinking and Its Application in Wood Coatings.

To broaden the applications of wood, it is necessary to prepare flame-retardant coatings that can protect wood substrates during combustion. In this study, a bio-based, intumescent, flame-retardant phytic acid-melamine polyelectrolyte (PM) was prepared using phosphorus-rich biomass phytic acid and nitrogen-rich melamine as raw materials through an ion crosslinking reaction. Subsequently, a series of bio-based, flame-retardant wood coatings were prepared by optimizing the structure of urea-formaldehyde resin with the addition of melamine, sodium lignosulfonate, and PM as a flame-retardant curing agent. Woods coated with PM-containing coatings displayed significantly improved flame-retardant performances in comparison to uncoated woods. For PM-cured woods, the measured values of total heat release and total smoke production were 91.51% and 57.80% lower, respectively, compared with those of uncoated wood. Furthermore, the fire growth index decreased by 97.32%, indicating a lower fire hazard. This increase in flame retardancy and smoke suppression performance is due to the dense expanded carbon layer formed during the combustion of the coating, which isolates oxygen and heat. In addition, the mechanical properties of the flame-retardant coatings cured with PM are similar to those cured with a commercial curing agent, NH4Cl. In addition, the prepared flame-retardant coating can also stain the wood. This study proves the excellent flame-retarding and curing effect of ammonium phytate in urea-formaldehyde resin coatings and provides a new approach for the application of bio-based flame retardants in wood coatings.

Optimization, characterization and evaluation of sodium alginate nanoparticles for Ganoderic acid DM encapsulation: Inhibitory activity on tyrosinase activity and melanin formation

The efficacy of nanoencapsulation as a technology for enhancing the solubility of active substances has been demonstrated. In this particular investigation, Ganoderic acid DM (GA-DM) was encapsulated within sodium alginate nanoparticles (NPs) using the ionic crosslinking method. The confirmation of the successful loading of GA-DM was ascertained through the analysis of Fourier transform infrared spectrum (FTIR). Empirical evidence derived from the examination of scanning electron microscope (SEM) images, transmission electron microscope (TEM) images, atomic force microscope (AFM) images, and dynamic light scattering (DLS) demonstrated a regular distribution and spherical morphology, with an average particle size of approximately 133 nm. The investigation yielded an encapsulation efficiency of 95.27 ± 0.11 % and a drug loading efficiency of 21.17 ± 0.02 % for the prepared sample. The release kinetics of SGPN was fitted with the Korsmeyer-Peppas kinetic model corresponding to diffusion-controlled release. The incorporation of GA-DM into sodium alginate nanocarriers exhibited a mitigating effect on the cytotoxicity of HaCat and B16, while also demonstrating inhibitory properties against tyrosinase activity and melanin formation.

Antibacterial Silver Nanoparticle Containing Polydopamine Hydrogels That Enhance Re-Epithelization.

A polydopamine polyelectrolyte hydrogel was developed by ionic crosslinking dextran sulfate with a copolymer of polyethyleneimine and polydopamine. Gelation was promoted by the slow hydrolysis of glucono-δ-lactone. Within this hydrogel, silver nanoparticles were generated in situ, ranging from 25 nm to 200 nm in size. The antibacterial activity of the hydrogel was proportional to the quantity of silver nanoparticles produced, increasing as the nanoparticle count rose. The hydrogels demonstrated broad-spectrum antibacterial efficacy at concentrations up to 108 cells/mL for P. aeruginosa, K. pneumoniae, E. coli and S. aureus, the four most prevalent bacterial pathogens in chronic septic wounds. In ex vivo studies on human skin, biocompatibility was enhanced by the presence of polydopamine. Dextran sulfate is a known irritant, but formulations with polydopamine showed improved cell viability and reduced levels of the inflammatory biomarkers IL-8 and IL-1α. Silver nanoparticles can inhibit cell migration, but an ex vivo human skin study showed significant re-epithelialization in wounds treated with hydrogels containing silver nanoparticles.

Spider-silk-inspired strong and tough hydrogel fibers with anti-freezing and water retention properties

Ideal hydrogel fibers with high toughness and environmental tolerance are indispensable for their long-term application in flexible electronics as actuating and sensing elements. However, current hydrogel fibers exhibit poor mechanical properties and environmental instability due to their intrinsically weak molecular (chain) interactions. Inspired by the multilevel adjustment of spider silk network structure by ions, bionic hydrogel fibers with elaborated ionic crosslinking and crystalline domains are constructed. Bionic hydrogel fibers show a toughness of 162.25 ± 21.99 megajoules per cubic meter, comparable to that of spider silks. The demonstrated bionic structural engineering strategy can be generalized to other polymers and inorganic salts for fabricating hydrogel fibers with broadly tunable mechanical properties. In addition, the introduction of inorganic salt/glycerol/water ternary solvent during constructing bionic structures endows hydrogel fibers with anti-freezing, water retention, and self-regeneration properties. This work provides ideas to fabricate hydrogel fibers with high mechanical properties and stability for flexible electronics.