Chitosan with different molecular weights (i.e., CS200 and CS2) as the ligand was employed to stabilize copper nanoclusters (CuNCs), developing a fluorescence “turn-on” probe to recognize fluoroquinolones. Chitosan chains not only can prevent the CuNCs from oxidation and overgrowth, but also provide the regulable luminescence and aggregation-induced emission (AIE) behaviors. The experimental results revealed that the CS200@CuNCs probe displayed better sensitivity, selectivity and anti-interference towards ciprofloxacin and several other specific fluoroquinolones than CS2@CuNCs. When recognizing the analytes, a more obvious AIE phenomenon occurred in CS200@CuNCs. The ciprofloxacin concentration for linear response was 1.0 180 µM, with a detection limit of 0.067 µM. Moreover, the CS200@CuNCs probe could be practically used to determine the ciprofloxacin residue from real samples with good recoveries, implying the perspective in various scenarios. These advantages are attributed to the flexile chain conformation for chitosan in CS200@CuNCs, which can generate the reasonable spatial-constraint. This structural feature significantly promotes the recognition and capture of target molecules. This work paves a distinctive way for designing novel biosensors by regulation of the ligand chain length, demonstrating high potential for rapid antibiotic screening.

Objective: To develop potential formulations for alleviating hyperuricemia, we screened approximately 10 medicinal and food homologous ingredients, including Apium graveolens L., Lycium ruthenicum Murray, and Inonotus obliquus, and explored their biological functions and underlying mechanisms. Methods: Based on the quantitative analysis from in vitro antioxidant capacity and xanthine oxidase inhibition for each candidate, the optimized formulation containing different ingredients, namely the homologous combinations 1 (FMHC1), could be obtained using the "Uniform Design Method". Further, the in vitro digestion behavior of FMHC1 was investigated. Besides, the protection efficiency on the hyperuricemia cell model that was established by inducing HK-2 cells with adenosine and xanthine oxidase was evaluated, by determining the levels of uric acid in cell supernatant, pro-inflammatory cytokines (IL-6, TNF-α), anti-inflammatory cytokines (IL-10, TGF-β), as well as the oxidative stress markers (MDA, CAT, SOD, GSH-Px). Results: The ideal formulation for FMHC1 was 41% Apium graveolens L., 39% Inonotus obliquus, 10% Lycium ruthenicum Murray, 5% Lonicera japonica Thunb, and 5% Stigma Maydis. The experimental results showed that FMHC1 displayed high bioavailability, where the inhibitory efficiency for xanthine oxidase was decreased by only 4.89%±1.02% (gastric phase) and 11.08%±1.59% (intestinal phase) after in vitro digestion. Moreover, the uric acid level in the hyperuricemia cell model was down-regulated by 35.52% by 1563 μg/mL FMHC1. These occurrences might be attributed to the ameliorated inflammatory responses through regulation of cytokines. Upon the administration, the IL-6 and TNF-α were downregulated by 25.82% and 66.51%, respectively, whereas the corresponding IL-10 and TGF-β were upregulated by 73.10% and 49.18%. Besides, the antioxidant capacity was significantly enhanced. As a result, about 61.20% loss for MDA level in cell line occurred, and the activities for CAT, SOD, and GSH-Px were enhanced by 2.86, 0.63, and 2.00 times, respectively. Conclusion: The screened FMHC1 demonstrates great potential in dealing with hyperuricemia through multiple pathways, and could be considered to be a promising diet in disease intervention.

The spontaneous self-organization of naturally-occurring polysaccharide particles into a thick and robust gel network at interface in Pickering emulsion is challenging. Inspired by the phenomenon that chitosan microgels (CSMs) with a certain size could self-associate into a solidified gel phase upon freezing, here we tentatively used CSMs to construct a highly-stable Pickering emulsion. CSMs can form a stable Langmuir's layer at the water/oil interface through the network deformation and re-arrangement of dangling chains, while the subsequent negative polymer coating can avoid the bridging resulting from the cross-association for CSMs on different emulsion droplets upon freezing. The experimental results indicated that the emulsion showed excellent features, including the wide pH range stability (3-12), long-term storage stability (>3 months), thermal stability (121 degrees C, 30 min). Moreover, CSMs could self-associate into a reliable gel layer around the oil droplet in freezing, leading to the better freeze-thaw stability (1-3 cycles). The negative coating not only facilitates the formation of interfacial gel network around each emulsion droplet, but also produces huge steric hindrance and electrostatic repulsion to suppress the coalescence. This work provides a different way to modulate the interfacial structure, thus developing a more stable polysaccharide-based Pickering emulsion.

OBJECTIVE:Hempseed threshing residues are rich in phytochemicals such as polyphenols and flavonoids. Phenolic and flavonoid compounds have been associated with antioxidant, antibacterial and anticancer activities. The re-use of the hempseed threshing residues as value-added materials is, not only cost-saving, but also environmentally beneficial. It is therefore important to develop an effective method for extraction of phenolic compounds and flavonoids from hempseed threshing residues. METHODS:In this investigation, the extraction of phenolic constituents and flavonoids from hempseed threshing residues using heat reflux extraction (HRE) were optimized through response surface methodology (RSM). Four HRE parameters to enhance the yield of crude extracts (CE), total phenolic content (TPC), and total flavonoids content (TFC) were evaluated. Additionally, the study evaluated the chemical compounds, antioxidant characteristics of the extracts, and the immune activity of the extracts was assessed by quantifying the levels of inflammatory cytokines, specifically IL-6, IL-10, and TNF-α. RESULTS:The best extraction parameters were determined as: for the extraction time of 69.71 min, a liquid-solid proportion of 5.12:1, a particle size of 1150 µm, and an ethanol concentration of 69.60%. Under these optimized conditions, the yields for CE, TPC, and TFC were 4.74%, 27.54%, and 16.02% respectively. The data conformed well to multiple regression models, showing that these extraction parameters markedly influence the yields of CE, TPC, and TFC. Most of the compounds found may belong to the class of polyphenol and flavonoids. Cellular assays indicated that extracts from hempseed threshing residue notably reduced pro-inflammatory factors (TNF-α, IL-6) and increased anti-inflammatory factors (IL-10) in RAW 264.7 cells. CONCLUSION:This research lays a theoretical foundation for extracting polyphenols and flavonoids from hempseed threshing residue and for the comprehensive assessment of antioxidant and immune-enhancing products. However, the antioxidant and immune activity of hempseed threshing residues extracts under physiological conditions in vivo, and the relevant mechanism should be further studied.

As one of the candidates for storage and conversion of new energy devices, zinc-air batteries have great advantages in terms of energy density/power density, safety, greenness, and cost. However, the slow kinetics of the oxygen reaction during the charging and discharging processes severely hinder the application of zinc-air batteries. This paper designs metal phosphides rationally to obtain a low-cost, highly efficient, and stable bifunctional catalyst Mn-CoFeP-2. The excellent performance of this catalyst for both the oxygen reduction reaction (ORR) and the oxygen evolution reaction (OER) is attributed to the doping of Mn, which optimizes the electronic structure of CoFeP and exposes more active sites. The Mn-CoFeP-2 catalyst exhibited excellent ORR performance (E onset = 0.853 V) and significantly enhanced OER electrocatalytic activity (overpotential of 443 mV at a current density of 10 mA cm-2). Density functional theory calculations show that the doping of Mn can effectively reduce the energy barrier of Co-Fe sites at the ORR and OER rate-limiting steps. In addition, the Mn-CoFeP-2-based rechargeable zinc-air battery can be cycled for 140 h at a current density of 2 mA cm-2, which exhibits a better cycling stability performance than the Pt/C-RuO2 battery (110 h). These outstanding results indicate that Mn-CoFeP-2 is a promising bifunctional catalyst for zinc-air batteries.

ObjectiveOligostilbenes, which have been associated with multiple biological activities, are a kind of oligomeric resveratrol compound and widely exist in Paeonia seeds threshing residues. The re-use of the Paeonia seeds threshing residues as value-added materials is, not only cost-effective, but also environmentally beneficial. It is therefore important to develop a high-efficiency method for extraction of oligostilbenes.MethodsIn this investigation, different extraction methods (soxhlet extraction, high temperature and pressure extraction, cold soaking extraction, heat reflux extraction, and ultrasonic extraction) were used to extract oligostilbenes from Paeonia seeds threshing residues. By comparing the extraction yield and in vitro antioxidant ability of oligostilbenes obtained from different extraction ways, the optimal extraction technology of Paeonia seeds threshing residues oligostilbenes was selected. The macroporous resin was used to purify oligostilbenes crude extract samples, and the purification conditions were determined. The protective effect of purified oligostilbenes on oxidative damage of MODE-K cells was evaluated.ResultsUltrasonic extraction with ethanol (UA-E) possessed the highest extraction yield of oligostilbenes, and the extraction yield was (3.45 ± 0.07)%. The oligostilbenes extracts obtained by different extraction methods had scavenging ability on DPPH· and ABTS+·, and UA-E showed relatively stronger scavenging ability at different concentration levels. The best resin for purifying oligostilbenes was X-5, and the adsorption and desorption rates were (93.12 ± 0.16)% and (91.33 ± 0.40)%, respectively. The optimal adsorption/desorption conditions were sample loading rate of 2 BV/h, ethanol concentration of 70%, and elution flow rate of 1.0 BV/h. There was a dose-response relationship between the scavenging ability of purified oligostilbenes on DPPH· and ABTS+· and the concentration of the samples. The oligostilbenes could relieve the oxidation effect of hydrogen peroxide (H2O2) on MODE-K cells, and enhance the protection of MODE-K cells by regulating the relative SOD activity, MDA, and ROS production.ConclusionThis research lays a theoretical foundation and scientific reference for the extraction, purification and application of Paeonia seed threshing residues in food and medicine.

Thermal dehydration, a common manufacturing process for structural materials, usually leads to the isotropic shrinkage of covalent hydrogels. Here, we reported a directional thermal dehydration process that generates strong anisotropic organization in chemically crosslinked chitosan hydrogels, providing a distinctive way to fabricate anisotropic soft matter without using any external force. In the dehydration, the preferred reorganization occurred from top surface and moved downwards, and the homogeneous polymer network was spontaneously transformed into stacked layers that were parallel to the dehydration surface. Scanning electron microscopic images combined with correlation function analysis revealed the obvious hierarchical structures across multiple length scales in hydrogel matrix. The resultant anisotropic hydrogel showed excellent mechanical properties, where the compressive strength and Young's modulus were enhanced by 10 similar to 15 and 20 similar to 110 times, respectively. Moreover, the lamellar structures with different directions can be well designed and integrated into a single hydrogel device in a controlled manner, thus addressing the delicate anisotropic architectures in three-dimensional biomimetic materials with any geometry.

Superhydrophilic hydrogel was typically used as the membrane coating on various substrates for oil/water separation. Nevertheless, these coatings may suffer from such limitations as poor adhesion strength and abrasionresistance. Thus, the facile construction of hydrogel sponge with 3D connecting channels would be an ideal choice. Herein, we reported a free-standing polyvinyl alcohol (PVA)/cellulose nanocrystal (CNC) hydrogel sponge for controllable oil/water separation. In the design, the salt/CNC hybrid crystals instead of conventional salt particles were employed as the sacrificial template, thus CNC was creatively integrated into the long and tortuous 3D interconnected channels via the solvent displacement combined template-leaching strategy. The resultant microstructure woven by CNC bundles in sponge channels could alleviate severe pore collapse in leaching process and oil intrusion. Moreover, it could serve as the superhydrophilic "sieve", promoting the separation efficiency significantly. The gravity-based separation efficiencies for PC5-HL hydrogel sponge in processing of diverse oil/water mixture and oil-in-water emulsions could achieve up to 99.7 and 99.4 %, respectively. In addition, this hydrogel sponge can be used for continuous oil/water separation without obvious decline upon several cycles. This work provides a different way to fabricate the eco-friendly, low-cost and energy-saving filtration hydrogel sponge, showing high potential in oily wastewater treatment.

To address the vulnerability of fruit during the storage period, an economical and green active film package is urgently required to extend the shelf life. In this work, a vanillin-derived dialdehyde (DV) was successfully synthesized, and further employed as the crosslink agent into chitosan matrix via the formation of Schiff base. The obtained film (CS-DV) with compact structure exhibited excellent stability, mechanical strength, barrier properties and bioactivities. The experimental results indicated that the tensile fracture stress was enhanced by 3.8-4.5 times in comparison with pure chitosan (CS) film. Due to the contained DV molecules, the UV irradiation in range of 250-400 nm was almost blocked by CS-DV films. Meanwhile, the diffuse of oxygen/water vapor across the CS-DV film were suppressed, preventing the dehydration and nutrient oxidation. Moreover, CS-DV films displayed high radical scavenging capacities, where the highest DPPH and ABTS radical scavenging ratios were evaluated to be 82.20% and 99.39%, respectively. In combination with their strong antibacterial activities against Staphylococcus aureus and Escherichia coli, CS-DV film package could significantly extend the shelf life of raspberry fruits with high preservation efficiency. This bio-based film only consists chitosan and vanillin derivative without any additives, showing potential as packaging material for agricultural and food products.

Polyvinyl alcohol (PVA) hydrogel as a hydrogel electrolyte faces issues such as fracture, dehydration, and poor conductivity, limiting its application in flexible zinc-air batteries. To address these, we propose a triethanolamine (TEA)-modified PVA-based hydrogel material (TPVA). TEA promoted formation of a uniform mesoporous structure and enables TPVA hydrogel to exhibit excellent mechanical properties, with an elongation at break (425

Direct methanol fuel cells (DMFCs), which utilize liquid methanol as fuel, exhibit a high energy density of 6.13 kWh/kg and low pollution emissions, are widely regarded as ideal "green" energy converters. However, electrocatalysts are poisoned by methanol dehydrogenation intermediates (CO) during methanol oxidation reaction (MOR) and oxygen reduction reaction (ORR), which inhibits electron transfer and slows reaction kinetics. Therefore, developing a high-performance, CO-tolerant bifunctional catalyst is crucial for achieving efficient and stable operation of DMFCs. In this study, synergistic active sites were generated through interaction of bimetallic composite oxides, thereby enhancing electron transfer efficiency and optimizing both MOR and ORR processes. Experimental results demonstrate that Cu1.5Co1.5O4 catalyst shows significant room for improvement, with its onset potential (Eonset = 0.857 V) and half-wave potential (E1/2 = 0.746 V) reaching 83 % of Pt/C catalysts. Demonstrating an outstanding current density of 75.76 mA cm-2 coupled with superior CO resistance. In DMFCs, it delivered a competitive power density of 20.45 mW cm-2. DFT calculations confirmed that composite oxide effectively regulates the binding energies of *CO and *OH intermediates, while notably reducing the overpotential in ORR theory. The changes in adsorption strength were further validated by d- and p-band center theory. This provides new design principles for the application of CuCo compositew oxides in DMFCs technology and clean energy systems.

While oral administration offers safety benefits, its therapeutic efficacy is hindered by various physiological factors within the body. In this study, a novel approach was explored using a matrix consisting of 2 % chitosan and 2 % gelatin, with citric acid (CA) serving as a green cross-linking agent (ranging from 0.4 % to 1.0 %), and curcumin (Cur) as the model drug to formulate hydrogel carriers. The results showed that a 0.4 % CA concentration, the hydrogel (CGA0.4) reached swelling equilibrium in deionized water within 40 min, exhibiting a maximum swelling index was 539 g/g. The addition of Cur to the CGA hydrogel (CGACur) notably enhanced release efficiency, particularly in simulated intestinal fluid, where Cur release rates exceeded 40 % within 100 min compared to below 8 % in other solutions. Among these hydrogels, CGA0.4Cur exhibited the fastest degradation rate in the combined solution, reaching >90 % degradation after 7 days. Additionally, Cur and CA demonstrated positive effects on the tensile strength, antioxidant activity and antibacterial activity of hydrogels. Compare to the bioaccessibility of CGC (27 %), those of CGACur had increased to over 34 %. These findings offer provide theoretical support for CA-crosslinked chitosan/gelatin gels in delivering hydrophobic bioactive molecules and their application in intestinal drug delivery system.

Rechargeable zinc-air batteries (ZABs) have been extensively studied due to their high energy and power density, high safety and cost-effectiveness, which are considered to be one of the most promising clean power sources in the field of energy storage. Nevertheless, its practical application has been hampered by the sluggish kinetics of the oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) during the discharge and charge processes, respectively. It is well known that Pt and IrO2 are currently considered to be the most efficient ORR and OER catalysts. However, the high cost of precious metal catalysts has hindered their large-scale application. Herein, a series of spinel catalysts (Mnx-Co3O4, x=0, 0.5, 1, 1.5) are prepared by co-precipitation method to achieve bifunctional oxygen electrocatalysis in alkaline media. Meanwhile, the potential of these transition metal oxide catalytic materials as bifunctional catalysts in replacing precious metals has been further explored. The results show that Mn-Co3O4 has excellent ORR performance (onset potential of 0.85 V, half-wave potential of 0.69 V), and significantly enhanced OER performance (overpotential of 0.57 V, the electron transfer resistance of 26.14 )), thereby leading to excellent bifunctional property. Furthermore, density functional theory (DFT) calculations synergistic effects in electrocatalytic processes. The characterization results further confirm that the doping of manganese in the catalyst preparation process increases the specific surface area and oxygen vacancies of the catalyst, adjusts the surface chemistry and electronic state of the catalyst, and thus improves the ORR and OER performance of the catalyst. In addition, the Mn-Co3O4 catalyst delivers high cycle life of up to 40 h in liquid rechargeable zinc air batteries. In summary, this work

Soft tissues, such as muscle could autonomously grow through re-alignment and/or -combination of collagen nanofibrils upon the mechanical training. This adaptive capability is highly expected in artificial materials, particularly in hydrogel actuator. In order to avoid the failure for devices by suffering from the accumulated mechanical loading, in this work, a double layered thermo-responsive hydrogel actuator capable of self-strengthening was successfully prepared. In the bilayer, PVA nanocrystals with different particle sizes were uniformly distributed in each monolayer matrix, giving rise to the asymmetric structure and the resultant differentiated de-swelling behaviors. Thus, the obtained hydrogel actuator with the semi-interpenetrating network of P(NIPAM-co-NMA) can display diverse programmable transformations by varying the temperatures. The existence of PVA nanocrystals in both layers not only can enhance the mechanical strength, dramatically minimizing the collapse of hydrogel actuator in service due to the imbalance of the mechanical properties for bilayer structure, but also was greatly involved in the self-reinforcing behavior. After repetitive tensile training with 80% strain, the tensile strength and fracture strain increased from 29.6 to 45.8 kPa and 95% to 104%, respectively. The experimental results indicated that the anisotropic orientation and strain-induced-crystallization for PVA crystalline domains readily occurred along the tensile direction, finally leading to the synchronous enhancement in mechanical strength for both layers. This work provides a new strategy for designing smart and robust biomimetic hydrogel systems that can be further used as the intelligent soft robotics in various fields.

Crystalline aggregates are widely present in various organisms. Regulation of nanostructures is of vital importance to the revelation of life secrets as well as material fabrication. As a representative, chitosan displays polymorphic structures. In tendon chitosan, four polymer chains are packed into an orthorhombic cell, where the antiparallel neighboring chains are linked by two sets of N-2O-6 hydrogen bonds, and water molecules are connected with N-2, O-3, and O-5 as well as O-6 atoms via hydrogen bonds to stabilize the hydrated structure. The transition from hydrated to anhydrous allomorphs, however, usually involved high-temperature annealing or multistep concentrated acid hydrolysis, which weakened the sustainability of chitosan. To address these issues, we proposed a more convenient strategy to achieve the polymorphic transitions under mild conditions. By subjecting chitosan microgels (CSM) to normal freezing treatment, the hydrated aggregates could be transferred into the anhydrous form. The X-ray diffraction (XRD) results clearly demonstrated that both the (020) and (200) diffraction peaks centered at 2 theta = 10 and 19.8 degrees gradually disappeared, while the (110) peak at 2 theta = 14.8 degrees indicated the occurrence of anhydrous crystals. Upon freezing, the water molecules that were inserted into the hydrated crystals were removed. Meanwhile, under the effects of N-2O-6 intermolecular hydrogen bonding and hydrophobic association, the adjacent polymer chains reorganized into new microcrystalline domains. Moreover, the CSM particles exhibited a strong tendency for self-association during this process. By introducing CSM into the oil/water mixture system to form a Pickering emulsion, the resultant macroporous materials could be used as the oil absorbent through subsequent lyophilization. This work provides a different way to facilely regulate the microcrystalline structure of chitosan in a controllable manner, facilitating the construction of more functional materials.

Bio-based food packaging materials have elicited growing interests due to their great degradability, high safety and active biofunctions. In this work, by simultaneously introducing the polyphenolic extracts from Capsicum annuum leaves and ferric ion (Fe3+) into the Polyvinyl alcohol/kappa-carrageenan (PVA/kappa-carrageenan)-based film-forming matrix, an active package film was developed, with the purpose to improve the food shelf life. The experimental results indicated that the existence of Fe3+ can not only improve the mechanical properties owing to the multiple dynamic coordinated interactions, but also endow the composite films with excellent fireretardancy. Moreover, the composite films could display excellent UV resistant performance, water vapor/oxygen gas barrier properties and antioxidant activities with the corporation of polyphenols. In particular, the highest DPPH and ABTS radical scavenging capacities for composite film (PC-PLP7 sample) were evaluated to be 82.5 % and 91.1 %, respectively. Higher polyphenol concentration is favorable to the bio-functions of the materials. Benefitting from these features, this novel kind of films with a dense and steady micro-structure could be further applicated in fruit preservations, where the ripening bananas were ensured with the high storage quality. This integration as a prospective food packaging material provides an economic and eco-friendly approach to excavate the high added-values of biomass.

Monitoring and recording subzero temperatures and humidity are essential activities for pharmaceutical, foodbeverage, and cold storage industries, as product quality can be hampered during storage and transportation due to temperature disruptions. Traditional electronic subzero time-temperature indicators (TTIs) can be energyinefficient, fragile, non-recyclable, and susceptible to data breaches and cyber-attacks. Hydrophilic colorimetric polymer nanofilms have been developed as colorimetric temperature and relative humidity (RH) sensors, however, the reversible color-changing behavior of these films significantly limited their application as TTIs, as cannot record temperature changes in the past. Herein, the first colorimetric polymer nanofilm-based TTI for recording an irreversible change of temperatures is reported. This device has shown quick color response in temperature ranges from 23 degrees C to -30 degrees C in fewer than 50 s. Remarkably, when the device experiences temperature disruption above a certain threshold time (t(th)), it shows irreversible color-changing behavior in response to the temperature change from subzero (-30 degrees C and -15 degrees C) to room temperature or above. It was demonstrated that tth, from minutes to days, of the TTI device can be precisely tuned by adjusting moisture absorber type and weight, interior RH, and storage temperature. Several field tests have demonstrated good versatility and applicability of the device.

Inspired by intelligent biomaterials which often have flexible responsiveness to multiple environmental cues and strengthen their mechanical properties by trainings, emerging soft actuators require programmable manipula-tion. Currently, the integration of such characteristics as rapid self-strengthening, strain-adaptive stiffening and smart actuation, into a single hydrogel actuator is urgently needed. Here, we report a self-strengthened hydrogel actuator based on the semi-interpenetrating polymer network consisting of polyvinyl alcohol (PVA) and poly(N-isopropylacrylamide) (PNIPAm), which can display diverse programmable actuations by responding to tem-perature/salt stimuli. In the design, the layer of freeze-thawed PNIPAm/PVA (PPGel-F) is assembled with another original PNIPAm/PVA hydrogel layer (PPGel) into one device. By taking advantage of the PVA crys-talline nanofibrils in the PPGel-F matrix, the differentiated swelling degree across the bilayer structure gives rise to asymmetric deformations and the resultant shape transformation. Moreover, upon the mechanical training with less than 100 cycles, the anisotropic arrangement of PVA nanofibrils through strong hydrogen bonding interactions can swiftly immobilize the amorphous polymer chains orientation along the tensile direction. This enhances the strain-induced crystallization, thereby generating the rapid self-strengthening behavior. The proposed work provides potential solution for constructing dynamically adaptive hydrogel systems that can mimic biological tissues for more intelligent soft robotics and bionic research.

The traditional x-carrageenan (xCG)-based hydrogel obtained from hot water can rupture easily under mechanical loading. To address this vulnerability, here we presented a robust all-xCG hydrogel without employing the second synthetic network. By simply regulating the polymer chains from random coil to stiff chain conformation in NaOH/urea solvent system via the freeze-thawing process, the as-prepared hydrogel with homogeneous structure can display an enhanced stretchability from 42.1 to 156 %, while maintaining the similar fracture stress. Moreover, upon the stepwise mechanical training and subsequent incubation in KCl aqueous solution, more helical segments of xCG were aligned and involved into the association domains, thus leading to the increment in both the crystallinity and anisotropy. Consequently, a fast self-strengthening behavior occurred, and a more stretchable (fracture strain up to 396 %), strong (stress 0.55 MPa) and tough (-1.52 MJ m-3) xCG hydrogel was obtained. In comparison to the traditional one, the fracture strain and toughness are increased by 8.5 and 11.5 times, respectively. In addition, this xCG hydrogel can demonstrate good recovery and shape memory behaviors under medium deformation. Hence, this tough all-xCG hydrogel is expected to be tailored into the biomaterials as the wearable device, artificial tendon, and cartilage in the future.