Natural Hydrogels Research Articles

Hydrogel Nanocomposite Towards Optical Sensing of Spermine in Biomedical and Real-Life Food Samples and Remediation of Toxic Dyes from Wastewater.

Nanocomposites such as graphene oxide (GO) have been incorporated into hydrogels to enhance conventional hydrogels' properties and develop new functions. Unique and strong molecular interactions between GO and low molecular weight gelators allow the fabrication of various functional hydrogels suitable for different applications. In the present study, we report a stable and soft nanocomposite hydrogel comprising a pyrene-based chiral amphipath having an amino acid (l-phenylalanine) core with pendant oligo-oxyethylene hydrophilic chains and GO. The mechanical and viscoelastic properties of the nanocomposite hydrogel were thoroughly studied using various spectroscopic, microscopic, and mechanical techniques. Even without GO, native hydrogels could form a self-supported thermoreversible and thixotropic hydrogel composed of the fibrillar network. Unlike native hydrogels, the morphological investigation of nanocomposite gels shows the presence of cross-linked nanosheet-like structures. The combined effect of π-π stacking and H-bonding interactions is the driving force for the formation of such composite hydrogels. Moreover, the nanocomposite hydrogels possess significantly superior mechanical stiffness than the native hydrogels. Interestingly, the thixotropic properties observed with the parent gel were retained even in the presence of carbon nanomaterials (GO). The nanocomposite hydrogel could be employed in the optical sensing of a biogenic polyamine, spermine, resulting in a visible gel-to-sol transition. The superior electrostatic interaction between the GOs and spermine molecules might have led to the release of entrapped fluorogenic dyes from the hydrogel network and a turn-on emission response. The sensory system was employed to analyze spermine content in human urine samples and decomposed food items. A gel-coated paper strip was also developed for onsite detection of the spermine. The nanocomposite hydrogel was further utilized to remove toxic organic dyes such as methylene blue (MB) and rhodamine B (RhB) from the aqueous media. The nanocomposite hydrogel thus showed excellent dye removal capabilities and was also found to be recyclable. Calculations of different mechanical parameters suggest that the dye removal efficiency of the nanocomposite hydrogel was better for MB than for RhB.

Growth Factor Immobilization to Synthetic Hydrogels: Bioactive bFGF-Functionalized Polyisocyanide Hydrogels.

With its involvement in cell proliferation, migration and differentiation basic fibroblast growth factor (bFGF) has great potential for tissue engineering purposes. So far, however, clinical translation of soluble bFGF-based therapies is unsuccessful, because the required effective doses are often supraphysiological, which may cause adverse effects. An effective solution is growth factor immobilization, whereby bFGF retains its bioactivity at increased efficacy. Studied carriers include films, solid scaffolds, and particles, as well as natural and synthetic hydrogels. However, these synthetic hydrogels poorly resemble the characteristics of the native extracellular matrix (ECM). In this work, bFGF is covalently conjugated to the synthetic, but highly biocompatible, polyisocyanide-based hydrogel (PIC-bFGF), which closely mimics the architecture and mechanical properties of the ECM. The growth factor conjugation protocol is straightforward and readily extrapolated to other growth factors or proteins. The PIC-bFGF hydrogel shows a prolonged bioactivity up to 4 weeks although no clear effects on the ECM metabolism are observed. Beyond the future potential of the PIC-bFGF hydrogel toward various tissue engineering applications, this work underlines that simple biological conjugation procedures are a powerful strategy to induce additional bioactivity in 3D synthetic cell culture matrices.

Natural polysaccharide-based hydrogel bioprinting for articular cartilage repair

Tissue engineering represents a promising approach for impaired articular cartilage tissue regeneration. 3D printed hydrogels have become an emerging tissue engineering strategy because they closely mimic the physical and biochemical characteristics of the extracellular matrix. The formulation of hydrogel ink holds significant importance in attaining a precisely defined scaffold, which could exhibit excellent shape fidelity post-printing. Natural polysaccharide-based hydrogels are a highly promising class of scaffold biomaterials for articular cartilage regeneration in the field of material science and tissue engineering. These hydrogels are particularly advantageous due to their exceptional water absorption capacity, biodegradability, adjustable porosity, and biocompatibility, which closely resemble those of the natural extracellular matrix. This review aims to provide a comprehensive overview of the key characteristics, functions, and research progress in 3D printing technology for natural polysaccharide-based hydrogels. Specifically, this review categorizes the commonly used natural polysaccharide-based hydrogel materials in cartilage tissue engineering, and summarizes the classic literature in this area. In the end, we provide a comprehensive analysis of the challenges and potential applications of natural polysaccharide-based hydrogels in cartilage tissue engineering.

Chitooligosaccharide reconstitutes intestinal mucus layer to improve oral absorption of water-soluble drugs

Intestinal mucus is a complex natural hydrogel barrier with unique physical properties that impede the absorption of various oral drugs. Both washout from the upper water layer and the physical resistance of the mucus layer particularly affect bioavailability of, especially, highly water-soluble molecules. One potential strategy for designing pharmaceutical formulations is to add absorption enhancers (AEs). However, there are few reports of AEs that work on mucus and their underlying mechanisms, leading to imprecise application. In this study, we investigated chitooligosaccharide (COS) as a safe, low-cost, and effective oral drug AE. We revealed the hydrodynamic law of interaction between COS and the intestinal mucus layer, which was associated with absorption benefiting mucus structural reconstruction. Based on this, we designed a translational strategy to improve the bioavailability of a group of soluble oral drugs by drinking COS solution before administration. Moreover, this research is expected to expand its application scenario by reducing drug dosage such as avoiding gastro-intestinal irritation and slowing veterinary antibiotic resistance.

Stretchable and sensitive sodium alginate ionic hydrogel fibers for flexible strain sensors

Ionic conductive hydrogel fibers based on natural polymers provide an immense focus for a new generation of electronics due to their flexibility and knittability. The feasibility of utilizing pure natural polymer-based hydrogel fibers could be drastically improved if their mechanical and transparent performances satisfy the requirements of actual practice. Herein, we report a facile fabrication strategy for significantly stretchable and sensitive sodium alginate ionic hydrogel fibers (SAIFs), by glycerol initiating physical crosslinking and by CaCl2 inducing ionic crosslinking. The obtained ionic hydrogel fibers not only show significant stretchability (tensile strength of 1.55 MPa and fracture strain of ∼161 %), but also exhibit wide-range sensing, satisfactorily stable, rapidly responsive, and multiply sensitive abilities to external stimulus. In addition, the ionic hydrogel fibers have excellent transparency (over 90 % in a wide wavelength range), and good anti-evaporation and anti-freezing properties. Furthermore, the SAIFs have been easily knitted into a textile, and successfully applied as wearable sensors to recognize human motions, by observing the output electrical signals. Our methodology for fabrication intelligent SAIFs will shed light on artificial flexible electronics and other textile-based strain sensors.

Natural Solid-State Hydrogel Electrolytes Based on 3D Pure Cotton/Graphene for Supercapacitor Application.

A conductive cotton hydrogel with graphene and ions can come into contact with electrodes in solid electrolytes at the molecular level, leading to a more efficient electrochemical process in supercapacitors. The inherently soft nature of cotton mixed with hydrogel provides superior flexibility of the electrolyte, which benefits the devices in gaining high flexibility. Herein, we report on the current progress in solid-state hydrogel electrolytes based on 3D pure cotton/graphene and present an overview of the future direction of research. The ionic conductivity of a complex hydrogel significantly increased by up to 13.9 × 10-3 S/cm at 25 °C, due to the presence of graphene, which increases ionic conductivity by providing a smooth pathway for the transport of charge carriers and the polymer. Furthermore, the highest specific capacitance of 327 F/g at 3 mV/s was achieved with cyclic voltammetry measurement and a galvanostatic charge-discharge measurement showed a peak value of 385.4 F/g at 100 mA/g current density. Furthermore, an electrochemical analysis demonstrated that a composite cotton/graphene-based hydrogel electrolyte is electrically stable and could be used for the design of next-generation supercapacitors.

Hydrogel for the Treatment of Osteoarthritis

Worldwide, the prevalence of osteoarthritis has grown significantly in recent years, and the rate of growth is accelerating. In recent years, the number of people with osteoarthritis has increased rapidly worldwide, and the rate of increase is on the rise. The development of osteoarthritis at an advanced stage can cause significant physical and psychological damage to patients. This article will introduce the application of natural and synthetic hydrogels in the field of osteoarthritis treatment. Natural hydrogels such as gelatin, alginate and polysaccharide have good biocompatibility and biodegradability and can be used for intra-articular drug delivery after modification. Synthetic hydrogels such as polyvinyl alcohol, polyethylene glycol and poly (lactic acid-hydroxyacetic acid) copolymer have good mechanical properties and can be used for intra-articular drug delivery and joint lubricants. In this article describes the application of hydrogels to carry a range of drugs and cell growth factors for the treatment of osteoarthritis, to act as scaffolds for cell growth, to lubricate joint cavities, and to reduce loads on joints, as well as several hydrogel modification methods to give them better biological or mechanical properties.

Engineered biomaterials to guide spheroid formation, function, and fabrication into 3D tissue constructs.

Cellular spheroids are aggregates of cells that are being explored to address fundamental biological questions and as building blocks for engineered tissues. Spheroids possess distinct advantages over cellular monolayers or cell encapsulation in 3D natural and synthetic hydrogels, including direct cell-cell interactions and high cell densities, which better mimic aspects of many tissues. Despite these advantages, spheroid cultures often exhibit uncontrollable growth and may be too simplistic to mimic complex tissue structures. To address this, biomaterials are being leveraged to further expand the use of cellular spheroids for biomedical applications. In this review, we provide an overview of recent studies that utilize engineered biomaterials to guide spheroid formation and function, as well as their fabrication into tissues for use as tissue models and for therapeutic applications. First, we describe biomaterial strategies that allow the high-throughput fabrication of homogeneously-sized spheroids. Next, we summarize how engineered biomaterials are introduced into spheroid cultures either internally as microparticles or externally as hydrogel microenvironments to influence spheroid behavior (e.g., differentiation, fusion). Lastly, we discuss a variety of biofabrication strategies (e.g., 3D bioprinting, melt electrowriting) that have been used to develop macroscale tissue models and implantable constructs through the guided assembly of spheroids. Overall, the goal of this review is to provide a summary of how biomaterials are currently being engineered and leveraged to support spheroids in biomedical applications, as well as to provide a future outlook of the field. STATEMENT OF SIGNIFICANCE: Cellular spheroids are becoming increasingly used as in vitro tissue models or as 'building blocks' for tissue engineering and repair strategies. Engineered biomaterials and their processing through biofabrication approaches are being leveraged to structurally support and guide spheroid processes. This review summarizes current approaches where such biomaterials are being used to guide spheroid formation, function, and fabrication into tissue constructs. As the field is rapidly expanding, we also provide an outlook on future directions and how new engineered biomaterials can be implemented to further the development of biofabricated spheroid-based tissue constructs.

Chitosan-based double network hydrogel loading herbal small molecule for accelerating wound healing

Skin injuries are one of the most common clinical traumas worldwide, and wound dressings are considered to be one of key factors in wound healing. Natural polymer-based hydrogels have been developed as ideal materials for a new generation of dressings due to their excellent biocompatibility and wetting ability. However, the inadequate mechanical performances and lack of efficacy in promoting wound healing have limited the application of natural polymer-based hydrogels as wound dressings. In this work, a double network hydrogel based on natural chitosan molecules was constructed to enhance the mechanical properties, and emodin, a herbal natural product, was loaded into the hydrogel to improve the healing effect of the dressing. The structure of the chitosan–emodin network formed by Schiff base reaction and microcrystalline network of biocompatible polyvinyl alcohol endowed hydrogels with excellent mechanical properties and ensured its integrity as wound dressings. Moreover, the hydrogel showed excellent wound healing properties due to the loading of emodin. The hydrogel dressing could promote cell proliferation, cell migration, and secretion of growth factors. The animal experimental results also demonstrated that the hydrogel dressing facilitated the regeneration of blood vessels and collagen and accelerated wound healing.

Accelerating the prediction and discovery of peptide hydrogels with human-in-the-loop

The amino acid sequences of peptides determine their self-assembling properties. Accurate prediction of peptidic hydrogel formation, however, remains a challenging task. This work describes an interactive approach involving the mutual information exchange between experiment and machine learning for robust prediction and design of (tetra)peptide hydrogels. We chemically synthesize more than 160 natural tetrapeptides and evaluate their hydrogel-forming ability, and then employ machine learning-experiment iterative loops to improve the accuracy of the gelation prediction. We construct a score function coupling the aggregation propensity, hydrophobicity, and gelation corrector Cg, and generate an 8,000-sequence library, within which the success rate of predicting hydrogel formation reaches 87.1%. Notably, the de novo-designed peptide hydrogel selected from this work boosts the immune response of the receptor binding domain of SARS-CoV-2 in the mice model. Our approach taps into the potential of machine learning for predicting peptide hydrogelator and significantly expands the scope of natural peptide hydrogels.

Self-Supporting Hyaluronic Acid-Functionalized G-Quadruplex-Based Perfusable Multicomponent Hydrogels Embedded in Photo-Cross-Linkable Matrices for Bioapplications.

Dynamic G-quadruplex supramolecular hydrogels have aroused great interest in a broad range of bioapplications. However, neither the development of native extracellular matrix (ECM)-derived natural biopolymer-functionalized G-quadruplex hydrogels nor their use to create perfusable self-supporting hydrogels has been explored to date, despite their intrinsic potential as carrier vehicles of therapeutic agents, or even living cells in advanced regenerative therapies, or as platforms to enable the diffusion of nutrients and oxygen to sustain long-term cell survival. Herein, we developed a dynamic co-assembling multicomponent system that integrates guanosine (G), 3-aminophenylboronic acid functionalized hyaluronic acid (HA-PBA), and potassium chloride to bioengineer strong, homogeneous, and transparent HA-functionalized G-quadruplex hydrogels with injectable, thermo-reversible, conductive, and self-healing properties. The supramolecular polymeric hydrogels were developed by hydrogen bonding and π-π stacking interactions between G coupled via dynamic covalent boronate ester bonds to HA-PBA and stabilized by K+ ions, as demonstrated by a combination of experiments and molecular dynamics simulations. The intrinsic instability of the self-assembled G-quadruplex structures was used to bioengineer self-supporting perfusable multicomponent hydrogels with interconnected size and shape-tunable hollow microchannels when embedded in 3D methacrylated gelatin supporting matrices. The microchannel-embedded 3D constructs have shown enhanced cell viability when compared to the bulk hydrogels, holding great promise for being use as artificial vessels for enabling the diffusion of nutrients and oxygen essential for cell survival. The proposed approach opens new avenues on the use of ECM-derived natural biopolymer-functionalized dynamic G-quadruplex hydrogels to design next-generation smart systems for being used in tissue regeneration, drug screening, or organ-on-a-chip.

Wearable Pressure Sensor Using Porous Natural Polymer Hydrogel Elastomers with High Sensitivity over a Wide Sensing Range.

Wearable pressure sensors capable of quantifying full-range human dynamic motionare are pivotal in wearable electronics and human activity monitoring. Since wearable pressure sensors directly or indirectly contact skin, selecting flexible soft and skin-friendly materials is important. Wearable pressure sensors with natural polymer-based hydrogels are extensively explored to enable safe contact with skin. Despite recent advances, most natural polymer-based hydrogel sensors suffer from low sensitivity at high-pressure ranges. Here, by using commercially available rosin particles as sacrificial templates, a cost-effective wide-range porous locust bean gum-based hydrogel pressure sensor is constructed. Due to the three-dimensional macroporous structure of the hydrogel, the constructed sensor exhibits high sensitivities (12.7, 5.0, and 3.2 kPa-1 under 0.1-20, 20-50, and 50-100 kPa) under a wide range of pressure. The sensor also offers a fast response time (263 ms) and good durability over 500 loading/unloading cycles. In addition, the sensor is successfully applied for monitoring human dynamic motion. This work provides a low-cost and easy fabrication strategy for fabricating high-performance natural polymer-based hydrogel piezoresistive sensors with a wide response range and high sensitivity.

Three-Dimensional Bioprinting of Naturally Derived Hydrogels for the Production of Biomimetic Living Tissues: Benefits and Challenges.

Three-dimensional bioprinting is the process of manipulating cell-laden bioinks to fabricate living structures. Three-dimensional bioprinting techniques have brought considerable innovation in biomedicine, especially in the field of tissue engineering, allowing the production of 3D organ and tissue models for in vivo transplantation purposes or for in-depth and precise in vitro analyses. Naturally derived hydrogels, especially those obtained from the decellularization of biological tissues, are promising bioinks for 3D printing purposes, as they present the best biocompatibility characteristics. Despite this, many natural hydrogels do not possess the necessary mechanical properties to allow a simple and immediate application in the 3D printing process. In this review, we focus on the bioactive and mechanical characteristics that natural hydrogels may possess to allow efficient production of organs and tissues for biomedical applications, emphasizing the reinforcement techniques to improve their biomechanical properties.

Hydrogels to Recapture Extracellular Matrix Cues That Regulate Vascularization.

The ECM (extracellular matrix) is a 3-dimensional network that supports cellular responses and maintains structural tissue integrity in healthy and pathological conditions. The interactions between ECM and cells trigger signaling cascades that lead to phenotypic changes and structural and compositional turnover of the ECM, which in turn regulates vascular cell behavior. Hydrogel biomaterials are a powerful platform for basic and translational studies and clinical applications due to their high swelling capacity and exceptional versatility in compositions and properties. This review highlights recent developments and uses of engineered natural hydrogel platforms that mimic the ECM and present defined biochemical and mechanical cues for vascularization. Specifically, we focus on modulating vascular cell stimulation and cell-ECM/cell-cell interactions in the microvasculature that are the established biomimetic microenvironment.

Plant-inspired adhesive and injectable natural hydrogels: invitroand invivo studies.

The development of alternative therapeutic treatments based on the use of medicinal and aromatic plants, such as Juniper communis L., has aroused interest in the medical field to find new alternatives to conventional therapeutic treatments, which have shown problems related to bacterial resistance, high costs, or sustainability in their production. The present work describes the use of hydrogels based on sodium alginate and carboxymethyl cellulose, with combinations of juniperus leaves and berry extracts, in order to characterize their chemical characteristics, antibacterial activity, tissue adhesion test, cytotoxicity in the L929 cell line, and their effects on an in vivo model in mice to maximize the use of these materials in the healthcare field. Overall, an adequate antibacterial potential against S. aureus, E. coli and P. vulgaris was obtained with doses above 100mg.mL-1 of hydrogels. Likewise, low cytotoxicity in hydrogels combined with extracts has been identified according to the IC50 value at 17.32µg.mL-1, compared to the higher cytotoxic activity expressed by the use of control hydrogels with a value at 11.05µg.mL-1. Moreover, in general, the observed adhesion was high to different tissues, showing its adequate capacity to be used in different tissue typologies. Furthermore, the invivo results have not shown erythema, edema, or other complications related to the use of the proposed hydrogels. These results suggest the feasibility of using these hydrogels in biomedical applications given the observed safety.

The Utilisation of Hydrogels for iPSC-Cardiomyocyte Research.

Cardiac fibroblasts' (FBs) and cardiomyocytes' (CMs) behaviour and morphology are influenced by their environment such as remodelling of the myocardium, thus highlighting the importance of biomaterial substrates in cell culture. Biomaterials have emerged as important tools for the development of physiological models, due to the range of adaptable properties of these materials, such as degradability and biocompatibility. Biomaterial hydrogels can act as alternative substrates for cellular studies, which have been particularly key to the progression of the cardiovascular field. This review will focus on the role of hydrogels in cardiac research, specifically the use of natural and synthetic biomaterials such as hyaluronic acid, polydimethylsiloxane and polyethylene glycol for culturing induced pluripotent stem cell-derived cardiomyocytes (iPSC-CMs). The ability to fine-tune mechanical properties such as stiffness and the versatility of biomaterials is assessed, alongside applications of hydrogels with iPSC-CMs. Natural hydrogels often display higher biocompatibility with iPSC-CMs but often degrade quicker, whereas synthetic hydrogels can be modified to facilitate cell attachment and decrease degradation rates. iPSC-CM structure and electrophysiology can be assessed on natural and synthetic hydrogels, often resolving issues such as immaturity of iPSC-CMs. Biomaterial hydrogels can thus provide a more physiological model of the cardiac extracellular matrix compared to traditional 2D models, with the cardiac field expansively utilising hydrogels to recapitulate disease conditions such as stiffness, encourage alignment of iPSC-CMs and facilitate further model development such as engineered heart tissues (EHTs).

Progress in the application of 3D-printed sodium alginate-based hydrogel scaffolds in bone tissue repair

In recent years, hydrogels have been widely used in the biomedical field as materials with excellent bionic structures and biological properties. Among them, the excellent comprehensive properties of natural polymer hydrogels represented by sodium alginate have attracted the great attention of researchers. At the same time, by physically blending sodium alginate with other materials, the problems of poor cell adhesion and mechanical properties of sodium alginate hydrogels were directly improved without chemical modification of sodium alginate. The composite blending of multiple materials can also improve the functionality of sodium alginate hydrogels, and the prepared composite hydrogel also has a larger application field. In addition, based on the adjustable viscosity of sodium alginate-based hydrogels, sodium alginate-based hydrogels can be loaded with cells to prepare biological ink, and the scaffold can be printed out by 3D printing technology for the repair of bone defects. This paper first summarizes the improvement of the properties of sodium alginate and other materials after physical blending. Then, it summarizes the application progress of sodium alginate-based hydrogel scaffolds for bone tissue repair based on 3D printing technology in recent years. Moreover, we provide relevant opinions and comments to provide a theoretical basis for follow-up research.

A new hydrogel to promote healing of bacteria infected wounds: Enzyme-like catalytic activity based on MnO2 nanocrytal

Manganese dioxide (MnO2) nanocrystal, a kind of nanomaterial with excellent enzyme-like catalytic properties, have been widely used in chemical, biological and pharmaceutical fields. It is composed of unique octahedral units that form a variety of tunnels and layered structures, which also lead to the emergence of different crystal forms and properties. In this study, different crystalline types of MnO2 were synthesized by different methods, and different substrates were used to study MnO2 catalytic ability of H2O2. β- MnO2 nanocrystal had nearly 50% oxygen, among which adsorbed oxygen accounted for nearly 65%, so it exhibited the best catalytic performance and could promote oxidation catalytic reaction well. Furthermore, a functional MnO2 hydrogel was prepared using β-MnO2 as antibacterial agent and natural gelatin hydrogel as carrier. The antibacterial performance of the new hydrogel was further studied, and the survival rate of different species of bacteria was<5% after high concentration of MnO2 functional hydrogel. In the end, MnO2 functional hydrogel was applied to the wound treatment of mice infected with antibiotic resistant bacteria, and it was found that the wound healing rate of mice was nearly 100% on the 14th day, indicating that it had the potential of a new antibacterial dressing.

Development of Natural Active Agent-Containing Porous Hydrogel Sheets with High Water Content for Wound Dressings

This work was concerned with the fabrication of a porous hydrogel system suitable for medium to heavy-exudating wounds where traditional hydrogels cannot be used. The hydrogels were based on 2-acrylamido-2-methyl-1-propane sulfonic acid (AMPs). In order to produce the porous structure, additional components were added (acid, blowing agent, foam stabilizer). Manuka honey (MH) was also incorporated at concentrations of 1 and 10% w/w. The hydrogel samples were characterized for morphology via scanning electron microscopy, mechanical rheology, swelling using a gravimetric method, surface absorption, and cell cytotoxicity. The results confirmed the formation of porous hydrogels (PH) with pore sizes ranging from ~50–110 µm. The swelling performance showed that the non-porous hydrogel (NPH) swelled to ~2000%, while PH weight increased ~5000%. Additionally, the use of a surface absorption technique showed that the PH absorbed 10 μL in &lt;3000 ms, and NPH absorbed &lt;1 μL over the same time. Incorporating MH the enhanced gel appearance and mechanical properties, including smaller pores and linear swelling. In summary, the PH produced in this study had excellent swelling performance with rapid absorption of surface liquid. Therefore, these materials have the potential to expand the applicability of hydrogels to a range of wound types, as they can both donate and absorb fluid.

A dual physical crosslinking starch-based hydrogel exhibiting high strength, fatigue resistance, excellent biocompatibility, and biodegradability.

Simultaneous realization of high strength, toughness, and fatigue resistance in natural starch-based hydrogel materials is challenging. A facile method of in situ self-assembly and a freeze-thaw cycle was proposed to construct double-network nanocomposite hydrogels of debranched corn starch/polyvinyl alcohol (Gels). Rheology, chemical structure, microstructure, and mechanical property of Gels were investigated. Notably, short linear starch chains were self-assembled into nanoparticles and subsequently into 3D microaggregates, which were tightly wrapped by starch and PVA network. Compared with corn starch single-network and starch/PVA double-network hydrogels, the Gels reached up to a higher compressive strength (ca. 1095.7kPa), and then achieved to ∼20-30-fold improvement in compressive strength. Recovery efficiency exceeded 85% after 20 successive compression loading-unloading cycle tests. Furthermore, the Gels had good biocompatibility to L929 cells. Hence, the high-performance starch hydrogels are thought to serve as a biodegradable and biocompatible material to replace synthetic hydrogels, which can broaden their application fields.