Homogeneous Hydrogels Research Articles

Exploration of silk-hyaluronic acid hydrogels crosslinked by the Fenton reaction

Herein, HRP-free silk-HA hybrid hydrogels are generated using the Fenton reaction. The findings reveal that a higher HA concentration, at an appropriate crosslinking density, increases the random coil content while decreasing the β-sheet content by reducing the interactions of Fe3+ ions with silk fibroin. This facilitates the formation of homogeneous hydrogel networks with enhanced optical transparency. The crosslinking strategies presented here offer a basis for the fabrication of hybrid hydrogel scaffolds based on proteins or polymers having phenolic hydroxyl moieties, without the use of HRP-catalyzed reactions, for a broad range of biomedical applications.

Synthesis and characterization of ultra-soft alginate hydrogel mimicking lung tissue

ABSTRACT Alginate hydrogels possess properties analogous to those of the extracellular matrix (ECM). Thus, their mechanical behavior approximates soft tissue, which makes them desirable for the production of tissue-equivalent soft deformable structures. This study aims to determine the synthesis-structure-property relationship for alginate hydrogel with the Young’s modulus in the range of 10°~101 kPa, mimicking to that of human lung tissue. Hydrogels, a 3D polymer network embedded in a water-rich environment. Homogeneous alginate hydrogels are synthesized by a direct mixture of sodium alginate and CaCO3, followed by the addition of D-glucono-δ-lactone (GDL) to initiate in-situ Ca2+ release and gelation. The influence of alginate concentration and molar ratio of the constituent calcium ion to carboxyl group from alginate monomer are evaluated while the Young’s modulus of the hydrogel is carefully controlled within the desired range. FTIR and SEM are used to characterize the influence of synthesis parameters at the molecular and microstructure levels. Tension and compression testing are performed to determine the Young’s modulus of the material. Empirical relations are established between synthesis parameters and the mechanical property. The result of the study will be subsequently used to guide the additive manufacturing of soft deformable structures based on alginate hydrogels.

Mechanical heterogeneity in a soft biomaterial niche controls BMP2 signaling

The extracellular matrix is known to impact cell function during regeneration by modulating growth factor signaling. However, how the mechanical properties and structure of biomaterials can be used to optimize the cellular response to growth factors is widely neglected. Here, we engineered a macroporous biomaterial to study cellular signaling in environments that mimic the mechanical stiffness but also the mechanical heterogeneity of native extracellular matrix. We found that the mechanical interaction of cells with the heterogeneous and non-linear deformation properties of soft matrices (E < 5 kPa) enhances BMP-2 growth factor signaling with high relevance for tissue regeneration. In contrast, this effect is absent in homogeneous hydrogels that are often used to study cell responses to mechanical cues. Live cell imaging and in silico finite element modeling further revealed that a subpopulation of highly active, fast migrating cells is responsible for most of the material deformation, while a second, less active population experiences this deformation as an extrinsic mechanical stimulation. At an overall low cell density, the active cell population dominates the process, suggesting that it plays a particularly important role in early tissue healing scenarios where cells invade tissue defects or implanted biomaterials. Taken together, our findings demonstrate that the mechanical heterogeneity of the natural extracellular matrix environment plays an important role in triggering regeneration by endogenously acting growth factors. This suggests the inclusion of such mechanical complexity as a design parameter in future biomaterials, in addition to established parameters such as mechanical stiffness and stress relaxation.

A Spontaneous In Situ Thiol-Ene Crosslinking Hydrogel with Thermo-Responsive Mechanical Properties.

The thermo-responsive behavior of Poly(N-isopropylacrylamide) makes it an ideal candidate to easily embed cells and allows the polymer mixture to be injected. However, P(NiPAAm) hydrogels possess minor mechanical properties. To increase the mechanical properties, a covalent bond is introduced into the P(NIPAAm) network through a biocompatible thiol-ene click-reaction by mixing two polymer solutions. Co-polymers with variable thiol or acrylate groups to thermo-responsive co-monomer ratios, ranging from 1% to 10%, were synthesized. Precise control of the crosslink density allowed customization of the hydrogel's mechanical properties to match different tissue stiffness levels. Increasing the temperature of the hydrogel above its transition temperature of 31 °C induced the formation of additional physical interactions. These additional interactions both further increased the stiffness of the material and impacted its relaxation behavior. The developed optimized hydrogels reach stiffnesses more than ten times higher compared to the state of the art using similar polymers. Furthermore, when adding cells to the precursor polymer solutions, homogeneous thermo-responsive hydrogels with good cell viability were created upon mixing. In future work, the influence of the mechanical micro-environment on the cell's behavior can be studied in vitro in a continuous manner by changing the incubation temperature.

Enhancing the supercapacitive performance of a carbon-based electrode through a balanced strategy for porous structure, graphitization degree and N,B co-doping

Regarding carbon-based electrodes, simultaneously establishing a well-defined meso-porous architecture, introducing abundant hetero-atoms and improving the graphitization degree can effectively enhance their capacitive performance. However, it remains a significant challenge to achieve a good balance between defects and graphitization degree. In this study, the porous structure and composition of carbon materials are co-optimised through a ‘dual-function’ strategy. Briefly, K3Fe(C2O4)3 and H3BO3 were hybridised with a gelatin aqueous solution to form a homogeneous composite hydrogel, followed by lyophilisation and carbonisation. Owing to the dual functionality of raw materials, the graphitization, activation and hetero-atom doping processes can occur simultaneously during a one-step high-temperature treatment. The resultant carbon material exhibits a high graphitization degree (ID/IG = 0.9 ± 0.1), high hetero-atom content (N: 9.0 ± 0.3 at.%, B: 6.9 ± 0.5 at.%) and a large specific area (1754 ± 58 m2/g). The as-prepared electrode demonstrates a superior capacitance of 383 ± 1F g−1 at 1 A/g. Interestingly, the cyclic voltammetry (CV) curves exhibit a distinctive pair of broad redox peaks, which is uncommon in KOH electrolyte. Experiment data and density functional theory (DFT) simulation verify that N-5, B co-doping enhances the activity of the faradic reaction of carbon electrodes in KOH electrolyte. Furthermore, the fabricated Zn-ion hybrid supercapacitor (ZHSC) based on this carbon electrode delivers a high-energy density of 140.7 W h kg−1 at a power density of 840 W kg−1.

Structural heterogeneity in tetra-armed gels revealed by computer simulation: Evidence from a graph theory assisted characterization.

Designing homogeneous networks is considered one typical strategy for solving the problem of strength and toughness conflict of polymer network materials. Experimentalists have proposed the hypothesis of obtaining a structurally homogeneous hydrogel by crosslinking tetra-armed polymers, whose homogeneity was claimed to be verified by scattering characterization and other methods. Nevertheless, it is highly desirable to further evaluate this issue from other perspectives. In this study, a coarse-grained molecular dynamics simulation coupled with a stochastic reaction model is applied to reveal the topological structure of a polymer network synthesized by tetra-armed monomers as precursors. Two different scenarios, distinguished by whether internal cross-linking is allowed, are considered. We introduce the Dijkstra algorithm from graph theory to precisely characterize the network structure. The microscopic features of the network structure, e.g., loop size, dispersity, and size distribution, are obtained via the Dijkstra algorithm. By comparing the two reaction scenarios, Scenario II exhibits an overall more idealized structure. Our results demonstrate the feasibility of the Dijkstra algorithm for precisely characterizing the polymer network structure. We expect this work will provide a new insight for the evaluation and description of gel networks and further help to reveal the dynamic process of network formation.

Superspreading of Polyelectrolyte Complex Solution for Constructing Hydrogel Coatings on Diverse Substrates

AbstractInjectable hydrogels have emerged as versatile materials with potential applications in various fields, including biomedicine, lubrication, adhesion, surface coatings, and tissue engineering. However, the critical aspect of spreading and wetting on various substrates, which is essential for obtaining significant interfacial properties, has not been adequately addressed. This work presents an approach to prepare hydrogel coatings on kinds of substrates through the superspreading of polyelectrolyte complex solution during its liquid‐liquid phase inversion process. Due to the low interfacial tension, the solution spreads and wets various surfaces underwater driven by osmotic pressure, improving the contact area and interface integration. Combined with the simultaneous sol‐gel transition through electrostatic interaction, it forms a stable and homogeneous hydrogel coating. The hydrogel coating possesses control thickness (4–8 µm), improved hydrophilicity (CA decrease from 102° to 10°), interfacial toughness (increase from 70 to 455 J m−2), and lubrication performance (coefficients of friction decrease from 0.712 to 0.112). The work provides an excellent opportunity to investigate the spreadability and wettability in a water/water/solid three‐phase system and develop functional hydrogel coatings for various applications.

Microinterfaces in biopolymer-based bicontinuous hydrogels guide rapid 3D cell migration

Cell migration is critical for tissue development and regeneration but requires extracellular environments that are conducive to motion. Cells may actively generate migratory routes in vivo by degrading or remodeling their environments or instead utilize existing extracellular matrix microstructures or microtracks as innate pathways for migration. While hydrogels in general are valuable tools for probing the extracellular regulators of 3-dimensional migration, few recapitulate these natural migration paths. Here, we develop a biopolymer-based bicontinuous hydrogel system that comprises a covalent hydrogel of enzymatically crosslinked gelatin and a physical hydrogel of guest and host moieties bonded to hyaluronic acid. Bicontinuous hydrogels form through controlled solution immiscibility, and their continuous subdomains and high micro-interfacial surface area enable rapid 3D migration, particularly when compared to homogeneous hydrogels. Migratory behavior is mesenchymal in nature and regulated by biochemical and biophysical signals from the hydrogel, which is shown across various cell types and physiologically relevant contexts (e.g., cell spheroids, ex vivo tissues, in vivo tissues). Our findings introduce a design that leverages important local interfaces to guide rapid cell migration.

Self-regulated reversal deformation and locomotion of structurally homogenous hydrogels subjected to constant light illumination

Environmentally adaptive hydrogels that are capable of reconfiguration in response to external stimuli have shown great potential toward bioinspired actuation and soft robotics. Previous efforts have focused mainly on either the sophisticated design of heterogeneously structured hydrogels or the complex manipulation of external stimuli, and achieving self-regulated reversal shape deformation in homogenous hydrogels under a constant stimulus has been challenging. Here, we report the molecular design of structurally homogenous hydrogels containing simultaneously two spiropyrans that exhibit self-regulated transient deformation reversal when subjected to constant illumination. The deformation reversal mechanism originates from the molecular sequential descending-ascending charge variation of two coexisting spiropyrans upon irradiation, resulting in a macroscale volumetric contraction-expansion of the hydrogels. Hydrogel film actuators were developed to display complex temporary bidirectional shape transformations and self-regulated reversal rolling under constant illumination. Our work represents an innovative strategy for programming complex shape transformations of homogeneous hydrogels using a single constant stimulus.

Highly oriented hydrogels for tissue regeneration: design strategies, cellular mechanisms, and biomedical applications.

Many human tissues exhibit a highly oriented architecture that confers them with distinct mechanical properties, enabling adaptation to diverse and challenging environments. Hydrogels, with their water-rich "soft and wet" structure, have emerged as promising biomimetic materials in tissue engineering for repairing and replacing damaged tissues and organs. Highly oriented hydrogels can especially emulate the structural orientation found in human tissue, exhibiting unique physiological functions and properties absent in traditional homogeneous isotropic hydrogels. The design and preparation of highly oriented hydrogels involve strategies like including hydrogels with highly oriented nanofillers, polymer-chain networks, void channels, and microfabricated structures. Understanding the specific mechanism of action of how these highly oriented hydrogels affect cell behavior and their biological applications for repairing highly oriented tissues such as the cornea, skin, skeletal muscle, tendon, ligament, cartilage, bone, blood vessels, heart, etc., requires further exploration and generalization. Therefore, this review aims to fill that gap by focusing on the design strategy of highly oriented hydrogels and their application in the field of tissue engineering. Furthermore, we provide a detailed discussion on the application of highly oriented hydrogels in various tissues and organs and the mechanisms through which highly oriented structures influence cell behavior.

Mechanical characterization of soft biomaterials: which time and spatial scale to choose?

The mechanical properties of soft gels hold significant relevance in biomedicine and biomaterial design, including the development of tissue engineering constructs and bioequivalents. It is important to adequately characterize the gel's mechanical properties since they play a role both in the overall structural properties of the construct and the physiological responses of cells. The question remains which approach for the mechanical characterization is most suitable for specific biomaterials. Our investigation is centered on the comparison of three types of gels and four distinct mechanical testing techniques: shear rheology, compression, microindentation, and nanoindentation by atomic force microscopy. While analyzing an elastic homogeneous synthetic hydrogel (a polyacrylamide gel), we observed close mechanical results across the different testing techniques. However, our findings revealed more distinct outcomes when assessing a highly viscoelastic gel (Ecoflex) and a heterogeneous biopolymer hydrogel (enzymatically crosslinked gelatin). To ensure precise data interpretation, we introduced correction factors to account for the boundary conditions inherent in many of the testing methods. The results of this study underscore the critical significance of considering both the temporal and spatial scales in mechanical measurements of biomaterials. Furthermore, they encourage the employment of a combination of diverse testing techniques, particularly in the characterization of heterogeneous viscoelastic materials such as biological samples. The obtained results will contribute to the refinement of mechanical testing protocols and advance the development of soft gels for tissue engineering.

Silk fibroin-based hemostatic powders with instant and robust adhesion performance for sutureless sealing of gastrointestinal defects.

Powder-based hemostatic technology has offered unprecedented opportunities in surgical sealing and repair of irregularly shaped and noncompressible wounds. Despite their routine use, existing clinical hemostatic powders are challenged either by poor mechanical properties or inadequate adhesion to bleeding tissues in biological environments. Here, inspired by the mussel foot proteins' fusion assembly strategy, a novel silk fibroin-based hemostatic powder (named as SF/PEG/TA) with instant and robust adhesion performance is developed. Upon absorbing interfacial liquids, the SF/PEG/TA powders rapidly swell into micro-gels and subsequently contact with each other to transform into a macroscopically homogeneous hydrogel in situ, strengthening its interfacial bonding with various substrates in fluidic environments. The in vitro and in vivo results show that the SF/PEG/TA powder possesses ease of use, good biocompatibility, strong antibacterial activities, and effective blood clotting abilities. The superior hemostatic sealing capability of the SF/PEG/TA powder is demonstrated in the rat liver, heart, and gastrointestinal injury models. Moreover, in vivo investigation of rat skin incision and gastrointestinal perforation models validates that the SF/PEG/TA powder promotes wound healing and tissue regeneration. Taken together, compared to existing clinical hemostatic powders, the proposed SF/PEG/TA powder with superior wound treatment capabilities has high potential for clinical hemostasis and emergency rescue.

Boosting Thermoelectric Performance of Thermogalvanic Hydrogels by Structure Engineering Induced by Liquid Nitrogen Quenching

AbstractQuasi‐solid thermogalvanic hydrogels hold great promise in harvesting low‐grade thermal energy, yet, they are still far from practical application owing to relatively low power output. Herein, through liquid nitrogen quenching‐induced structure engineering, a high‐performance stretchable thermogalvanic hydrogel thread with a high specific output power density of 2227.5 µW m−2 K−2 and a large thermopower of 4.5 mV K−1 is designed. After liquid nitrogen quenching, both the thermopower and electrical conductivity have been greatly improved compared to natural cooling. The excellent properties are attributed to liquid nitrogen quenching‐induced grain refinement and precipitation inhibition. It is a novel and general preparation method for high‐performance and homogeneous thermogalvanic hydrogels. Finally, a thermogalvanic hydrogel array is demonstrated to be capable of driving a low‐power motor and charging a mobile phone by low‐grade thermal energy harvesting, indicating a great potential for practical applications in human daily life.

Oriented Self-assembly of Flexible MOFs Nanocrystals into Anisotropic Superstructures with Homogeneous Hydrogels Behaviors.

Building of metal-organic frameworks (MOFs) homogeneous hydrogels made by spontaneous crystallization remains a significant challenge. Inspired by anisotropically structured materials in nature, an oriented super-assembly strategy to construct micro-scale MOFs superstructure is reported, in which the strong intermolecular interactions between zirconium-oxygen (Zr─O) cluster and glutamic acid are utilized to drive the self-assembly of flexible nanoribbons into pumpkin-like microspheres. The confined effect between water-flexible building blocks and crosslinked hydrogen networks of superstructures achieved a mismatch transformation of MOFs powders into homogeneous hydrogels. Importantly, the elastic and rigid properties of hydrogels can be simply controlled by precise modulation of coordination and self-assembly for anisotropic superstructure. Experimental results and theoretical calculations demonstrates that MOFs anisotropic superstructure exhibits dynamic double networks with a superior water harvesting capacity (119.73gg-1) accompanied with heavy metal removal (1331.67mgg-1) and strong mechanical strength (Young's modulus of 0.3GPa). The study highlights the unique possibility of tailoring MOFs superstructure with homogeneous hydrogel behavior for application in diverse fields.

3D-bioprinted anisotropic bicellular living hydrogels boost osteochondral regeneration via reconstruction of cartilage–bone interface

Reconstruction of osteochondral (OC) defects represents an immense challenge due to the need for synchronous regeneration of special stratified tissues. The revolutionary innovation of bioprinting provides a robust method for precise fabrication of tissue-engineered OCs with hierarchical structure; however, their spatial living cues for simultaneous fulfilment of osteogenesis and chondrogenesis to reconstruct the cartilage-bone interface of OC are underappreciated. Here, inspired by natural OC bilayer features, anisotropic bicellular living hydrogels (ABLHs) simultaneously embedding articular cartilage progenitor cells (ACPCs) and bone mesenchymal stem cells (BMSCs) in stratified layers were precisely fabricated via two-channel extrusion bioprinting. The optimum formulation of the 7% GelMA/3% AlgMA hydrogel bioink was demonstrated, with excellent printability at room temperature and maintained high cell viability. Moreover, the chondrogenic ability of ACPCs and the osteogenic ability of BMSCs were demonstrated invitro, confirming the inherent differential spatial regulation of ABLHs. In addition, ABLHs exhibited satisfactory synchronous regeneration of cartilage and subchondral bone invivo. Compared with homogeneous hydrogels, the neo-cartilage and neo-bone in ABLHs were augmented by 23.5% and 20.8%, respectively, and more important, a more harmonious cartilage-bone interface was achieved by ABLHs due to their well-tuned cartilage-bone-vessel crosstalk. We anticipate that such a strategy of tissue-mimetic ABLH by means of bioprinting is capable of spatiotemporal cell-driven regeneration, offering insights into the fabrication of anisotropic living materials for the reconstruction of complex organ defects.

Tailoring Homogeneous Hydrogel Nanospheres by Facile Ultra-Sonication Assisted Cross-Linked Copolymerization for Rhodamine B Dye Adsorption.

The present paper describes the design of shape-oriented hydrogel nanospheres using a facile ultrasonication-supported crosslinked copolymerization technique. The effect of variable monomer concentration on the homogeneity of hydrogel nanospheres was investigated. The chitosan-cl-poly(MMA) hydrogel nanospheres were well characterized using various techniques such as FTIR, XRD, TGA, SEM, and TEM. The chitosan-cl-poly(MMA) hydrogel nanospheres were studied for their swelling behavior and could potentially be used as a novel adsorbent for rhodamine B dye remediation from aqueous media. The study found that utilizing chitosan-cl-poly(MMA) nanohydrogel spheres at the optimal pH 5 increased RhB dye adsorption capacity from 7.9 to 17.8 mg/g (pH 2 to 5), followed by a slight reduction. Furthermore, when nanohydrogel concentration increased, adsorption capacity dropped from 18.03 to 2.8 mg/g, but adsorption percentage climbed from 90.2% to 97.8%. At an initial dye concentration of 140 mg/L, rhodamine B adsorption achieved 204.3 mg/g in 60 min. The rhodamine B dye adsorption study includes adsorption kinetics, isotherm, and thermodynamics analyses. The interpretation of the adsorption study revealed that Langmuir isotherms fit best with a qmax value of 276.26 mg/g, which is in close approximation with the experimental value, whereas pseudo-second-order kinetics explains the adsorption process rate. The interaction of RhB dye with chitosan-cl-poly(MMA) hydrogel nanospheres involves multiple forces such as electrostatic interactions, hydrogen bonding, van der Waals forces, etc.

Laser-guided programmable construction of cell-laden hydrogel microstructures for in vitro drug evaluation

Cell-laden hydrogel microstructures have been used in broad applications in tissue engineering, translational medicine, and cell-based assays for pharmaceutical research. However, the construction of cell-laden hydrogel microstructures in vitro remains challenging. The technologies permitting generation of multicellular structures with different cellular compositions and spatial distributions are needed. Herein, we propose a laser-guided programmable hydrogel-microstructures-construction platform, allowing controllable and heterogeneous assembly of multiple cellular spheroids into spatially organized multicellular structures with good bioactivity. And the cell-laden hydrogel microstructures could be further leveraged for in vitro drug evaluation. We demonstrate that cells within hydrogels exhibit significantly higher half-maximal inhibitory concentration values against doxorubicin compared with traditional 2D plate culture. Moreover, we reveal the differences in drug responses between heterogeneous and homogeneous cell-laden hydrogel microstructures, providing valuable insight into in vitro drug evaluation.

Road Narrow-Inspired Strain Concentration to Wide-Range-Tunable Gauge Factor of Ionic Hydrogel Strain Sensor.

The application of stretchable strain sensors in human movement recognition, health monitoring, and soft robotics has attracted wide attention. Compared with traditional electronic conductors, stretchable ionic hydrogels are more attractive to organization-like soft electronic devices yet suffer poor sensitivity due to limited ion conduction modulation caused by their intrinsic soft chain network. This paper proposes a strategy to modulate ion transport behavior by geometry-induced strain concentration to adjust and improve the sensitivity of ionic hydrogel-based strain sensors (IHSS). Inspired by the phenomenon of vehicles slowing down and changing lanes when the road narrows, the strain redistribution of ionic hydrogel is optimized by structural and mechanical parameters to produce a strain-induced resistance boost. As a result, the gauge factor of the IHSS is continuously tunable from 1.31 to 9.21 in the strain range of 0-100%, which breaks through the theoretical limit of homogeneous strain-distributed ionic hydrogels and ensures a linear electromechanical response simultaneously. Overall, this study offers a universal route to modulate the ion transport behavior of ionic hydrogels mechanically, resulting in a tunable sensitivity for IHSS to better serve different application scenarios, such as health monitoring and human-machine interface.

Growth factor-loaded sulfated microislands in granular hydrogels promote hMSCs migration and chondrogenic differentiation.

Cell-based therapies for articular cartilage lesions are expensive and time-consuming; clearly, a one-step procedure to induce endogenous repair would have significant clinical benefits. Acellular heterogeneous granular hydrogels were explored for their injectability, cell-friendly cross-linking, and ability to promote migration, as well as to serve as a scaffold for depositing cartilage extracellular matrix. The hydrogels were prepared by mechanical sizing of bulk methacrylated hyaluronic acid (HAMA) and bulk HAMA incorporating sulfated HAMA (SHAMA). SHAMA's negative charges allowed for the retention of positively charged growth factors (GFs) (e.g., TGFB3 and PDGF-BB). Mixtures of HAMA and GF-loaded SHAMA microgels were annealed by enzymatic cross-linking, forming heterogeneous granular hydrogels with GF deposits. The addition of GF loaded sulfated microislands guided cell migration and enhanced chondrogenesis. Granular heterogeneous hydrogels showed increased matrix deposition and cartilage tissue maturation compared to bulk or homogeneous granular hydrogels. This advanced material provides an ideal 3D environment for guiding cell migration and differentiation into cartilage. STATEMENT OF SIGNIFICANCE: Acellular materials which promote regeneration are of great interest for repair of cartilage defects, and they are more cost- and time-effective compared to current cell-based therapies. Here we develop an injectable, granular hydrogel system which facilities cell migration from the surrounding tissue, facilitating endogenous repair. The hydrogel architecture and chemistry were optimized to increase cell migration and extracellular matrix deposition. The present study provides quantitative data on the effect of microgel size and chemical modification on cell migration, growth factor retention and tissue maturation.

Hydrogel‐Based Flexible Energy Storage Using Electrodes Based on Polypyrrole and Carbon Threads

AbstractDeveloping new flexible and electroactive materials is a significant challenge to producing safe, reliable, and environmentally friendly energy storage devices. This study introduces a promising electrolyte system that fulfills these requirements. First, polypyrrole (PPy) nanotubes are electropolymerized in graphite‐thread electrodes using methyl orange (MO) templates in an acidic medium. The modification increases the conductivity and does not compromise the flexibility of the electrodes. Next, flexible supercapacitors are built using hydrogel prepared from poly(vinyl alcohol) (PVA)/sodium alginate (SA) obtained by freeze–thawing and swollen with ionic solutions as an electrolyte. The material exhibits a homogenous and porous hydrogel matrix allowing a high conductivity of 3.6 mS cm−1 as‐prepared while displaying great versatility, changing its electrochemical and mechanical properties depending on the swollen electrolyte. Therefore, it allows its combination with modified graphite‐thread electrodes into a quasi‐solid electrochemical energy storage device, achieving a specific capacitance (Cs) value of 66 F g−1 at 0.5 A g−1. Finally, the flexible device exhibits specific energy and power values of 19.9 W kg−1 and 3.0 Wh kg−1, relying on the liquid phase in the hydrogel matrix produced from biodegradable polymers. This study shows an environment friendly, flexible, and tunable quasi‐solid electrolyte, depending on a simple swell experiment to shape its properties according to its application.