Swelling Capacity Of Hydrogels Research Articles

Synthesis and characterization of an innovative sodium alginate/polyvinyl alcohol bioartificial hydrogel for forward-osmosis desalination.

Recently, hydrogels have been widely applied as draw agents in forward osmosis (FO) desalination. This work aims to synthesize bioartificial hydrogel from a blend of sodium alginate (SA) and polyvinyl alcohol (PVA) using epichlorohydrin (ECH) as a crosslinker. Then this prepared hydrogel was applied as a draw agent with cellulose triacetate membrane in a batch (FO) cell. The effects of the PVA content in the polymer blend and the crosslinker dose on the hydrogel's swelling capacity were investigated to optimize the hydrogel's composition. Furthermore, the water flux and the reverse solute flux of the optimum SA/PVA hydrogel were evaluated in a batch (FO) unit under the effect of the hydrogel's particle size, feed solution (FS) temperature, FS concentration, and membrane orientation. Fourier transform infrared spectroscopy (FTIR), scanning electron microscopy (SEM), X-ray diffraction (XRD) and compression strength tests were used to characterize the prepared hydrogel. Results revealed that the equilibrium swelling ratio (%) of 5228 was achieved with a hydrogel that had 25% PVA and a crosslinking ratio of 0.8. FO experiments revealed that the maximum water flux of 0.845 LMH achieved, when distilled water was used as FS, average hydrogel's particle size was 60µm, and the FS temperature was 40°C.

Heparinized Acellular Hydrogels for Magnetically Induced Wound Healing Applications.

The control of angiogenesis has the potential to be used for regulation of several pathological and physiological processes, which can be instrumental on the development of anticancer and wound healing therapeutical approaches. In this study, mesenchymal stem/stromal cells (MSCs) were seeded on magnetic-responsive gelatin, with or without heparin functionalization, and exposed to a static 0.08 T magnetic field (MF), for controlling their anti-inflammatory and angiogenic activity, with the aim of accelerating tissue healing. For the first time, it was examined how the amount of heparin and magnetic nanoparticles (MNPs) distributed on gelatin scaffolds affected the mechanical properties of the hydrogels and the morphology, proliferation, and secretome profiling of MSCs. The findings demonstrated that the addition of MNPs and heparin affects the hydrogel swelling capacity and renders distinct MSC proliferation rates. Additionally, MF acts as a topographical cue to guide MSCs alignment and increases the level of expression of specific genes and proteins that promote angiogenesis. The results also suggested that the presence of higher amounts of heparin (10 μg/cm3) interferes with the secretion and limits the capacity of angiogenic factors to diffuse through the hydrogel and into the culture medium. Ultimately, this study shows that acellular heparinized hydrogels efficiently retain the angiogenic growth factors released by magnetically stimulated MSCs thus rendering superior wound contraction (55.8% ± 0.4%) and cell migration rate (49.4% ± 0.4%), in comparison to nonheparinized hydrogels (35.2% ± 0.7% and 37.8% ± 0.7%, respectively). Therefore, these heparinized magnetic hydrogels can be used to facilitate angiogenesis in various forms of tissue damage including bone defects, skin wounds, and cardiovascular diseases, leading to enhanced tissue regeneration.

Preparation and Characterization of Bovine Small Intestine Submucosa (SIS) ‎Hydrogel

The aim of this study was to prepare and characterize a small intestine submucosa (SIS) hydrogel as ‎a bio-scaffold. In this study, SIS from five calves, aged 8-12 months and weighing 250-300 kg, was ‎obtained from a slaughterhouse immediately after slaughtering. The SIS was then decellularized, ‎powdered, and subsequently transformed into a hydrogel. This transformation was achieved by ‎dissolving the decellularized SIS powder in phosphate-buffered saline (PBS) at a concentration of ‎‎50% w/v, and allowing it to form a hydrogel over a 12-hour period at 37 °C. Characterization of the ‎SIS hydrogel was conducted using various techniques. Fourier Transform Infrared Spectroscopy ‎‎(FTIR) was employed to identify the chemical structure of the hydrogel, revealing three primary peaks ‎at 1639 cm-1, 1571 cm-1, and 1338 cm-1, corresponding to amide I, II, and III bands, respectively. ‎Additionally, a broad signal at 3440 cm-1 was observed, indicative of the hydroxyproline side chain. ‎The hydrogel's swelling capacity was evaluated, showing an expansion of 437% after a 12-hour ‎immersion in PBS at a pH of 7.4. Scanning Electron Microscopy (SEM) analysis of the lyophilized ‎hydrogel revealed a highly porous and interconnected architecture, resembling a honeycomb ‎structure. Moreover, the hydrogel's antibacterial efficacy was assessed against Staphylococcus ‎aureus using an agar diffusion test, which demonstrated a zone of inhibition measuring 16.11 mm. ‎The combined chemical, morphological, and antibacterial properties of the SIS hydrogel developed ‎in this study suggest its potential as a promising bio-scaffold for inducing tissue regeneration and ‎restoring tissue function‎.

Aloe vera Rind Valorization to Improve the Swelling Capacity of Commercial Acrylic Hydrogels

Acrylic hydrogels have been used in agriculture to increase the availability of water in the soil; cause faster plant growth and increase plant survival to water stress; allow controlled release of fertilizers; and, therefore, increase crop yields. On the other hand, Aloe vera gel production generates a large amount of solid waste as cuticles, which is currently underutilized despite that it is a good source of cellulose nanofibers that could be used to improve the swelling capacity of commercial acrylic hydrogels. In this work, both morphology (SEM) and particle size (TEM) of the cellulose nanofibers obtained from A. vera cuticles by the acid hydrolysis method combined with ultrasound were analyzed; as well as the presence of functional groups (FITR) and thermal stability (TGA). Then, acrylic hydrogels were synthesized by the solution polymerization method, and nanofibers were added to these hydrogels at different concentrations (0% w w−1, 3% w w−1, 5% w w−1, and 10% w w−1). These concentrations had a nonlinear relationship with the swelling capacity, and the hydrogel reinforced at 3% cellulose nanofiber was chosen as the best formulation in this work, as this one improved the swelling capacity of hydrogels at equilibrium (476 g H2O g hydrogel−1) compared to the hydrogel without nanofiber (310 g H2O g hydrogel−1), while hydrogels with 10% nanofiber had a similar swelling capacity to the non-reinforced hydrogel (295 H2O g hydrogel−1). Therefore, cellulose-based superabsorbent hydrogels with potential application in agriculture were developed in this work.

Enhanced Macroporous Cationic Chitosan Hydrogel by Freezing and Thawing Method with Superadsorption Capacity for Anionic Dyes

In this study, we have developed a simple technique to prepare cationic chitosan hydrogel with interconnected porous structure using freeze–thaw process and the obtained hydrogel was named FCS hydrogel. Scanning electron microscopy (SEM) imaging discovered that the synthesized hydrogel demonstrated interconnected porous structure in the scope of 5–20 μm. We also showed that the FCS hydrogel exhibits pH responsiveness behavior, and demonstrated reversible swelling and de-swelling behaviors maintaining their mechanical stability. We demonstrate that the FCS hydrogel swelling capacity decreased at alkaline pH and rose with a decline in pH value. Besides, the FCS hydrogel presented specific surface area of 78.25 ± 8.75 m2 g−1, due to the cryogenic treatment of glutaraldehyde cross-linked chitosan hydrogel could increase the surface area and permeability of composite hydrogel and then strongly increasing the adsorption capacity. Subsequently, the FCS monolithic hydrogel tested dyes removal, which provides a high removal efficiency towards anionic dyes including congo red (CR) and sodium fluorescein (SFL) dyes. Significantly, we show that the FCS hydrogel could be regenerated and reused as an adsorbent for wastewater treatment without significant loss of pollutants removal efficiency over a number of adsorption and washing cycles. This study offers a promising environmental friendly and sustainable interconnected porous hydrogel for anionic dye removal from wastewater.

Gels based on calcium alginate/pillared bentonite: structural characterization and their use as cadmium removal agent

In this work, calcium alginate hydrogels with natural and pillared bentonites (0.5 and 5% w/w) were synthetized in two geometries (disks and beads) and their capacity to adsorb cadmium ion from aqueous media was evaluated. Pillarization effect on bentonite morphology was evidenced by SEM, XRD, LD and BET isotherms. Structure and swelling capacity of hydrogels were determined, showing that hydrogels beads with pillared clays presented the higher ability to retain water. Regarding cadmium adsorption capacity, the effect of pH media (3, 5 and 7), the contact time (0 to 320 min.) and the initial cadmium ion concentration (6 to 42 mg/L) were studied employing hydrogel beads. Regardless bentonite type and concentration, the optimal pH cadmium adsorption was 7, reaching the highest adsorption capacity (93%) for hydrogel with 0.5% natural bentonite. Besides, the equilibrium adsorption time was reached at 120 min for all studied hydrogels and experimental data fitted with a pseudo-second order kinetic model.

Kinetics of methylene blue dye adsorptive removal using halloysite nanocomposite hydrogels

Abstract In the present work, halloysite nano-clay (HNTs) based hydrogel was fabricated and their efficiency for the removal of methylene blue dye was studied. The hydrogel films were prepared with varying amount of halloysite nano-clay via facile solution casting method. Effect of halloysite clay on adsorption performance of composite was investigated. The hydrophobic thermoplastic synthetic polymer, polylactic acid (PLA) was blended with hydrophilic polymer polyvinyl alcohol (PVA) and HNTs to synthesize hydrogels. Swelling behavior and antimicrobial efficiency was also evaluated. The halloysite incorporating films showed excellent antibacterial activity. Swelling capacity of hydrogel with increased halloysite content was reduced due to increased crosslinking among polymer chains. Halloysite incorporated hydrogel exhibited higher adsorption ability as compared to film comprising of only PVA and PLA and dye removal followed pseudo first order kinetics. Film with 0.03 g HNTs rapidly attained adsorption-desorption equilibria and removed the dye completely within 30 min. Results confirmed that synthesized film could be potentially used for the removal of cationic dye and fabricated hydrogel film have promising potential for wastewater treatment since a higher adsorption capacity was observed for halloysite nano-clay incorporated hydrogel.

Chemo-mechanical modelling of swelling and crosslinking reaction kinetics in alginate hydrogels: A novel theory and its numerical implementation

Hydrogels are mechanically stabilized through the action of external agents which induce the formation of crosslinks in the polymer network as a consequence of transport and reactive mechanisms. Crosslinking increases the stiffness of the construct, produces inelastic deformations in the polymer network and interacts with the swelling capacity of hydrogels. The control of this process is hence crucial for fulfilling functional criteria in several technological fields, like drug-delivery or bioprinting. Nevertheless, experimental approaches for monitoring the crosslinking kinetics with the required resolution are currently missing. The development of new computational models in the field might open the way to novel investigation tools. This paper presents a thermodynamically consistent chemo-mechanical model in large deformation for reactive–diffusive mechanisms occurring during crosslinking in alginate hydrogels. The system accounts for shrinking and swelling effects, fluid movements, as well as the reaction kinetics of calcium-induced crosslinking. Crosslinks alter mechanical and diffusive properties in the hydrogel. Moreover, on the basis of thermodynamic arguments, internal stresses directly affect the crosslinking kinetics, revealing a two-way coupling between mechanics and chemistry. The model is implemented in a finite element framework, considering a monolithic coupling between chemical transport and mechanics. The computational framework allows characterizing the (experimentally inaccessible) heterogeneous distribution of mechano-chemical quantities and properties in the hydrogel. Parametric campaigns of simulations are presented to investigate hydrogels’ behaviour and compare numerical outcomes with available experimental evidence.

Synthesis and absorption properties of hybrid polyacrylamide hydrogels

Hydrogel absorbents were synthesized based on cross-linking of Polyacrylamide grafted on Dextran or Dextran sulfate sodium salt. It was found that the swelling capacity of hydrogels depends on cross-linker concentration as well as Dextran component. FT-IR studies of hydrogels were carried out to analyze its structure. Methylene blue dye as model cationic medical drug was applied for the absorption/desorption study. Hybrid hydrogels prove the mechanism of absorption by the formation of charged polyelectrolyte/dye complexes. The kinetic model of pseudo-first order was applied to determine the rate constant k of the reaction between hydrogels and dye in the solution.

Antibacterial Properties and pH Sensitive Swelling of Insitu Formed Silver-Curcumin Nanocomposite Based Chitosan Hydrogel.

A simple method was used to prepare curcumin/silver nanocomposite based chitosan hydrogel. In an alkaline medium, chitosan and chitosan nanocomposite hydrogels were prepared using the physical crosslinking method. The prepared hydrogels were stable for a long period at room temperature. In one step, silver nanoparticles were prepared insitu using silver nitrate solution and curcumin oxide within the hydrogel network formation. In the meantime, curcumin compound served as both a reducing and stabilizing agent. The structure and surface morphology of nanocomposite hydrogels were characterized by FTIR, SEM, and EDX analysis confirmed the formation of silver nanoparticles within the hydrogel network. Moreover, Images of TEM showed a spherical shape of silver nanoparticles with an average size of 2–10 nm within the matrix of the hydrogel. The formation mechanism of nanocomposite based hydrogel was reported. Besides that, the effect of chitosan and silver nitrate concentrations were studied. The swelling capacity of the prepared nanocomposite hydrogels was also performed at different pH of 4, 7, and 9. From the experimental results, the swelling capacity of hydrogels depends on the concentrations of chitosan and silver nitrate. The prepared composite based hydrogel exceeds a higher swelling degree than chitosan hydrogels at low pH. The antibacterial activity of the nanocomposite hydrogels was also examined; the results showed that the prepared nanocomposite hydrogels outperformed the pure chitosan hydrogels. This shows them to be a promising material for the biomedical field as a wound dressing and drug release.

Synthesis and characterization of poly(vinyl alcohol)/chondroitin sulfate composite hydrogels containing strontium-doped hydroxyapatite as promising biomaterials.

Novel poly(vinyl alcohol)/chondroitin sulfate (PVA/CS) composite hydrogels containing hydroxyapatite (HA) or Sr-doped HA (HASr) particles were synthesized by a freeze/thaw method and characterized aiming towards biomedical applications. HA and HASr were synthesized by a wet-precipitation method and added to the composite hydrogels in fractions up to 15 wt%. Physical-chemical characterizations of particles and hydrogels included scanning electron microscopy, energy-dispersive spectroscopy, Fourier-transform infrared spectroscopy, X-ray diffraction, thermogravimetry, porosity, compressive strength/elastic modulus, swelling degree, and cell viability. Particles were irregular in shape and appeared to have narrow size variation. The thermal behavior of composite hydrogels was altered compared to the control (bare) hydrogel. All hydrogels exhibited high porosity. HA/HASr particles reduced total porosity without reducing pore size. The mechanical strength was improved as the fraction of HA or HASr was increased. HASr particles led to a faster water uptake but did not interfere with the total hydrogel swelling capacity. In cell viability essay, increased cell growth (above 120%) was observed in all groups including the control hydrogel, suggesting a bioactive effect. In conclusion, PVA/CS hydrogels containing HA or HASr particles were successfully synthesized and showed promising morphological, mechanical, and swelling properties, which are particularly required for scaffolding.

The synthesizing of different hydrogel nanocarriers for oral insulin delivery

Diabetes is seen as the global health problem of the world due to the high risk of complications and the increasing prevalence of death. The routine diagnosis of diabetes is the injection of insulin. This treatment has a lot of side effects known to the patient (infection at injection sites, irritation, etc.). In order to overcome such conditions in the treatment of diabetes and provide faster recovery, many different delivery systems for insulin are being studied. Hydrogels are interesting polymers with hydrophobic structure that can be designed in 3D networks for oral insulin delivery. In this study, we studied the synthesis of biodegradable, biocompatible, low-toxicity therapeutic hydrogels. Acrylamide (ACR):carboxymethyl cellulose (CMC) (ACR/CMC), Acrylamide (ACR): Chitosan (Chi) and Chitosan:glutaraldehyde hydrogels were prepared. The CMC was used in acrylamide-based hydrogels for both comonomer and biocompatibility. The swelling capacity of hydrogels and the in vitro release of insulin from hydrogels were studied at different pH. Insulin release studies have shown that ACR/CMC hydrogels are a good and new alternative as an oral insulin carrier.

Cross-linked xanthan gum–starch hydrogels as promising materials for controlled drug delivery

The work was intended to develop a novel acrylic acid grafted hydrogel by chemical crosslinking of xanthan gum and starch under microwave irradiation. The swelling capacity of hydrogel was found to be dependent upon pH. The maximum swelling capacity of hydrogel was recorded as 32.21 g/g under the optimized conditions. The swelling capacity of hydrogel was quite higher than most of the hydrogels containing xanthan gum mentioned in the literature. Various characterization techniques including FTIR, SEM, TGA and XRD confirmed successful synthesis of hydrogel with porous morphology and better thermal stability. Synthesized hydrogel was employed as an oral drug delivery vehicle. Releasing behavior of the hydrogels for the drugs aspirin and paracetamol was studied under specific physiological conditions. The drug release was significantly higher at pH 7.4 in comparison to acidic and neutral media. Synthesized hydrogel was found to be suitable for colon-specific drug delivery. Both aspirin and paracetamol followed non-Fickian diffusion mechanism at higher pH and Fickian mechanism at lower pH. Release profiles of both the drugs were best fitted in the first order model. Hydrogel was found to be non-cytotoxic to human fibroblast cells and biocompatible, with a low hemolytic ratio. Consequently results supported potential of this non-toxic, biofriendly and appropriately tailored polysaccharide based hydrogel to be used as drug delivery carrier for controlled and site-specific drug release.

Formulation and evaluation of interpenetrating network of xanthan gum and polyvinylpyrrolidone as a hydrophilic matrix for controlled drug delivery system

The prime objective of the present study was to develop novel colon targeting xanthan gum/polyvinylpyrrolidone-co-poly acrylic acid hydrogels for controlled delivery of 5-fluorouracil at colon-specific site by combining the properties of natural and synthetic polymers. Xanthan gum (XG) and polyvinylpyrrolidone (PVP) polymer have been chemically cross-linked with acrylic acid (AA) monomer using ethylene glycol dimethacrylate and ammonium per sulfate/sodium hydrogen sulfite as a cross-linker and initiator, respectively. Different proportions of XG, PVP, acrylic acid and ethylene glycol dimethacrylate were blended with each other to fabricate pH-sensitive hydrogels by free radical polymerization. SEM, FTIR, TGA, DSC, XRD and sol−gel fraction analysis were carried out for characterization and structural analysis of polymeric system. pH-responsive behavior of fabricated hydrogels was investigated by performing swelling studies and in vitro drug release studies at both pH 1.2 and pH 7.4. Toxicity studies were performed on rabbits to evaluate cytotoxicity and biocompatibility. TGA and DSC confirmed that formulations were thermodynamically stable, while FTIR, SEM and XRD revealed the successful grafting of components. By increasing the content of polymer, monomer and cross-linker, gel fraction was found to be increased. Swelling capacity of hydrogels increases with the increase in concentration of monomer, while swelling capacity tends to decreases with the increase in concentration of cross-linker and polymer in hydrogel composition. pH sensitivity of hydrogels was confirmed by swelling dynamic and drug release behavior in simulated gastrointestinal fluids. Toxicity studies confirmed that hydrogels were non-toxic. Drug release kinetics revealed the controlled release pattern of 5-fluorouracil in developed polymeric network. Cross-linked XG/PVP-co-poly (AA) hydrogels can be used as promising candidate for controlled delivery of 5-FU for prolonged treatment period at colon-specific site.

Bi-functional silica nanoparticles for simultaneous enhancement of mechanical strength and swelling capacity of hydrogels

A combination of strong load-bearing capacity and high swelling degree is desired in hydrogels for many applications including drug delivery, tissue engineering, and biomedical engineering. However, a compromising relationship exists between these two most important characteristics of hydrogels. Improving both of these important properties simultaneously in a single hydrogel material is still beyond the satisfactory limit. Herein, we report a novel approach to address this problem by introducing a silica-based bi-functional 3D crosslinker. Our bi-functional silica nanoparticles (BF-Si NPs) possess amine groups that are able to offer pseudo-crosslinking effects induced by inter-cohesive bonding, and acrylate groups that can form conventional covalent crosslinking in the same hydrogel. We fabricated polyacrylic acid (PAc-Si) and polyacrylamide (PAm-Si) hydrogels using our BF-Si NPs via free radical polymerization to demonstrate this concept. Incorporation of the BF-Si crosslinkers into the hydrogels has resulted in a large enhancement in the mechanical properties compared to conventional hydrogel crosslinked with N,N′-methylene bisacrylamide (MBA). For instance, tensile strength and the toughness increased by more than 6 times and 10 times, respectively, upon replacing MBA with BF-Si in polyacrylamide hydrogel. Moreover, the hydrogels crosslinked with BF-Si exhibited a remarkably elevated level of swelling capacity in the aqueous medium. Our facile yet smart strategy of employing the 3D bi-functional crosslinker for combining high swelling degree and strong mechanical properties in the same hydrogels can be extended to the fabrication of many similar acrylate or vinyl polymer hydrogels.

A Novel pH- and Salt-Responsive N-Succinyl-Chitosan Hydrogel via a One-Step Hydrothermal Process.

In this study, we synthesized a series of pH-sensitive and salt-sensitive N-succinyl-chitosan hydrogels with N-succinyl-chitosan (NSCS) and the crosslinker glycidoxypropyltrimethoxysilane (GPTMS) via a one-step hydrothermal process. The structure and morphology analysis of the NSCS and glycidoxypropyltrimethoxysilane-N-succinyl chitosan hydrogel (GNCH) revealed the close relation between the swelling behavior of hydrogels and the content of crosslinker GPTMS. The high GPTMS content could weaken the swelling capacity of hydrogels and improve their mechanical properties. The hydrogels show high pH sensitivity and reversibility in the range of pH 1.0 to 9.0, and exhibit on-off switching behavior between acidic and alkaline environments. In addition, the hydrogels perform smart swelling behaviors in NaCl, CaCl2, and FeCl3 solutions. These hydrogels may have great potential in medical applications.

Hybrid chitosan/amniotic membrane-based hydrogels for articular cartilage tissue engineering application

A hybrid hydrogel combining collagen and chitosan (Ch) and human amniotic membranes (AM) were produced. To produce hybrid hydrogels, a fixed concentration of chitosan (2%) was used, adding AM as a booster at the concentrations of 2.5, 5.0. and 10.0% (w/w). DSC curves showed the denaturation of collagen. The swelling capacity of hydrogels ranged between 333 ± 19% and 368 ± 28%. The groups Ch-1.0 mg/mL and Ch-2.0 mg/mL had an elastic modulus 27% higher than the other groups.

Methylene blue removal by using pectin-based hydrogels extracted from dragon fruit peel waste using gamma and microwave radiation polymerization techniques

This research aims to compare the ability of smart hydrogel in removing the methylene blue prepared by using two different radiation methods. The extracted pectin from the dragon fruit peel (Hylocereus polyrhizus) was used with acrylic acid (AA) to produce a polymerized hydrogel through gamma and microwave radiation. The optimum hydrogel swelling capacity was obtained by varying the dose of radiation, pectin to AA ratio and pH used. From the array of samples, the ideal hydrogel was obtained at pH 8 with a ratio of 2:3 (pectin: AA) using 10 kGy and 400 W radiated gamma and microwave respectively. The performance of both hydrogels namely as Pc/AA(G) (gamma) and Pc/AA(Mw) (microwave) were investigated using methylene blue (MB) adsorption studies. In this study, three variables were manipulated, pH and MB concentration and hydrogel mass in order to find the optimum condition for the adsorption. Results showed that 20 mg of Pc/AA(G) performed the highest MB removal which was about 45% of 20 mg/L MB at pH 8. While 30 mg of Pc/AA(Mw) able to remove up to 35% of 20 mg/L MB at the same pH condition. To describe the adsorption mechanism, both kinetic models pseudo-first-order, pseudo-second-order were employed. The results from kinetic data showed that it fitted the pseudo-first-order as compared to pseudo-second-order model equation. This study provides alternative of green, facile and affective biomaterial for dye absorbents that readily available.

Hybrid polyacryamide hydrogels: Synthesis, properties and prospects of application

Hybrid hydrogels based on polyacrylamide were prepared by using N,N’-methylene-bis-acrylamide as cross-linker during radical polymerization of two component Dextran/Acrylamide system. It was found that the swelling capacity of hydrogels depends on cross-linker concentration as well as Dextran component. SEM, TGA and DSC studies of hybrid polyacryamide hydrogels were carried out to analyze its structure. Hydrogels were tested as wound dressings. Proposed hydrogels could keep proper moisture balance and a programmed acid-alkaline equilibrium on the wound surface.

Nanocellulose reinforced gellan-gum hydrogels as potential biological substitutes for annulus fibrosus tissue regeneration

Intervertebral disc (IVD) degeneration is associated with both structural damage and aging related degeneration. Annulus fibrosus (AF) defects such as annular tears, herniation and discectomy require novel tissue engineering strategies to functionally repair AF tissue. An ideal construct will repair the AF by providing physical and biological support, facilitating regeneration. The presented strategy herein proposes a gellan gum-based construct reinforced with cellulose nanocrystals (nCell) as a biological self-gelling AF substitute. Nanocomposite hydrogels were fabricated and characterized with respect to hydrogel swelling capacity, degradation rate in vitro and mechanical properties. Rheological evaluation on the nanocomposites demonstrated the GGMA reinforcement with nCell promoted matrix entanglement with higher scaffold stiffness observed upon ionic crosslinking. Compressive mechanical tests demonstrated compressive modulus values close to those of the human AF tissue. Furthermore, cell culture studies with encapsulated bovine AF cells indicated that nanocomposite constructs promoted cell viability and a physiologically relevant cell morphology for up to fourteen days in vitro.