Janus Hydrogel Research Articles

Mussel-inspired thermo-switchable underwater adhesive based on a Janus hydrogel

On-demand underwater adhesives with excellent adhesive and gentle detachment properties enable stable connections to various biomedical devices and biointerfaces and avoid the risk of harmful tissue damage upon detachment. Herein, we present a Janus hydrogel adhesive that can reversibly switch its adhesion strength, which is controlled by temperature, using a thermoresponsive polymer and mussel-inspired molecules. This thermoswitchable adhesive (TSA) hydrogel displays both strong adhesion and gentle detachment with an over 1000-fold gap in underwater adhesion strength onto glass, titanium, aluminum, and Teflon substrates when exposed to temperatures above and below the lower critical solution temperature (LCST). The adhesion switch is possibly caused by the change in toughness of the TSA hydrogels with temperature because the Janus hydrogel possesses gradient crosslinked structures. Moreover, the lowermost surface is sufficiently soft to gently detach from the substrate below the LCST. The electrode-integrated hydrogel remains on human skin, and electrical signals are continuous over 10 min above the LCST. In contrast, commercially available hydrogel electrodes quickly swell and detach from the skin. The thermoswitchability of the TSA hydrogel, with its robust adhesion and gentle detachment, offers significant potential for biomedical applications characterized by minimally invasive procedures.

Asymmetric Wettability Hydrogel Surfaces for Enduring Electromyographic Monitoring.

Hydrogel electrode interfaces have shown tremendous promise in the acquisition of surface electromyography (EMG) signals. However, the perspiration or moisture environments will trigger the deadhesion between hydrogel electrodes and human skin. Despite the hydrophobic/hydrophilic surfaces can perform the anti-moisture or adhesion respectively, it remains a challenge to integrally form a Janus hydrogel with homogeneous mechanical elasticity and electronic performance. Herein, a surface induction strategy is proposed to approach the hydrophobic/hydrophilic hydrogel surfaces. The hydrophobic interaction between surfactants and molds regulates the distribution of hydrophobic/hydrophilic monomers on the surface. The hydrophobic molds induce a hydrophilic hydrogel surface, while the hydrophilic molds induce a hydrophobic surface. It presents a new phenomenon of reversal wettability inducing and optional hydrogel surfaces. The integral Janus hydrogel can be easily obtained by the hydrophilic molds. Balance of adhesion, elasticity, and conductivity endows the hydrogel electrode patch with durable conformal adhesion and high-fidelity EMG signals even in the sweaty epidermis due to the asymmetric wettability surfaces. This hydrogel performs the quantitative description of muscle strength and accurate fatigue assessment. It offers a reliable candidate for future practical applications in continuous digital healthcare and intelligent human-machine interaction, even the Metaverse.

A bio-inspired Janus hydrogel patch facilitates oral ulcer repair by combining prolonged wet adhesion and lubrication

Oral ulcers, the most common type of mucosal lesion, are both highly prevalent and prone to recurrence. In the persistently moist environment of the oral cavity, current therapeutic patches face challenges such as short adhesion time, disruption by food particles and bacteria, and oral movements. To address these challenges, we develop a Janus patch, named ANSB, inspired by the multi-layered and asymmetric structure of natural mucosa, featuring a long-lasting adhesive layer and a lubricating layer. By eliminating the salivary barrier and leveraging covalent crosslinking between tissue surface amine groups and N-hydroxysuccinimide ester (NHS), the adhesive layer—composed of gelatin and acrylic acid—achieves rapid (≤ 30 s), strong (≥ 45 kPa), and durable (≥ 8 h) adhesion to wet buccal tissues. Furthermore, the efficient lubricating effect (COF = 0.02 ± 0.003) provided by zwitterions renders the lubricating layer of ANSB highly similar to natural mucosal tissue, effectively preventing bacterial invasion, secondary damage, and unintended adhesion. Additionally, the strong interlayer bonding and complementary mechanical properties are confirmed, resulting in a unified performance characterized by rapid wet adhesion, hydration lubrication, and enhanced mechanical strength. Importantly, ANSB treatment demonstrates a long-term protective barrier and superior therapeutic effects in rat oral ulcers, inhibiting pseudomembrane formation and accelerating tissue regeneration without causing secondary damage. Consequently, this distinctive Janus patch, characterized by prolonged adhesion, efficient lubrication, and simple preparation, holds significant potential for clinical oral ulcer treatment. Statement of SignificanceOral ulcers, with healing impeded by secondary injury and bacterial invasion due to the absence of protective barriers, are highly prevalent and recurrent. However, sustaining therapeutic materials and physical barriers in the highly dynamic and moist oral environment poses a considerable challenge. In this study, a Janus patch (ANSB) that integrated a soft wet adhesive layer and a tough lubricating layer was developed to reconstruct a new protective barrier thus preventing external stimuli such as secondary damage and bacterial infiltration. This innovative patch with high therapeutic potential for oral ulcers may offer a new way for ulcer treatment based on barrier protection.

Biocompatible chitin-based Janus hydrogel membranes for periodontal repair

Periodontal defects caused by severe periodontitis are a widespread issue globally. Guided tissue regeneration (GTR) using barrier membranes for alveolar bone repair is a common clinical treatment. However, most commercially available collagen barrier membranes are expensive and lack the antibacterial properties essential for effective bone regeneration. Herein, we report a natural polysaccharide chitin hydrogel barrier membrane with a Janus structure (ChT-PDA-p-HAP), featuring high antibacterial and protein-repelling activity on the outer side and good osteogenesis ability on the inner side. This multifunctional membrane is fabricated though a three-step process: (i) dissolution and regeneration of chitin, (ii) co-deposition with polydopamine (PDA) and poly(sulfobetaine methacrylate) (pSBMA), and (iii) coating with gelatin-hydroxyapatite (gelatin-HAP). In vitro cell experiments demonstrated the membrane's high biocompatibility and significant osteogenic activity. In vivo implantation in rats with periodontal defects revealed that the cemento-enamel junction index of the ChT-PDA-p-HAP membrane (1.165 mm) was superior to that of the commercial Bio-Gide® membrane (1.350 mm). This work presents a method for fabricating a chitin-based Janus barrier membrane, potentially expanding the use of chitin in tissue engineering. Statement of significanceThis study introduces a Janus hydrogel membrane based on chitin, tailored for guided tissue regeneration in periodontal defects. By combining antibacterial properties and osteogenic capabilities in a single membrane, the ChT-PDA-p-HAP membrane represents a significant advancement over traditional collagen barriers. Its outer surface, enhanced by Cu2+ and PDA-pSBMA coatings, resists bacterial colonization and protein adhesion effectively, while the inner side, coated with gelatin-HAP, promotes robust bone formation. In vitro experiments demonstrate high biocompatibility and substantial osteogenic differentiation, while in vivo testing in rat models confirms good therapeutic efficacy compared to commercial membranes. This multifunctional approach not only utilizes chitin's abundant natural resource but also integrates simple coating techniques to enhance therapeutic outcomes in periodontal tissue engineering, offering promising avenues for broader biomedical applications.

Tough and anisotropic Janus hydrogel for tendon injury repair with controlled release of bFGF in tendon microenvironment

To address the high complexity and challenging nature of large-scale tendon injury repair, an innovative Janus structured hydrogel patch (JAHP@bFGF) was designed in this study. The patch combines microenvironmental responsiveness with efficient repair function, aiming to optimise and accelerate the tendon healing process. The outer layer is a PVA/SA/Na3Cit hydrogel with excellent mechanical properties, protein resistance, and low friction, which provides firm support to the tendon and reduces adhesions to ensure the recovery of gliding function. The inner layer of TCSB@bFGF microgel responds intelligently to changes in the microenvironment, precisely regulates the release of bFGF, promotes cell proliferation and migration, accelerates tissue regeneration, and has high adhesion strength and antimicrobial properties, which significantly reduces the risk of postoperative infection. Experimental results show that JAHP@bFGF significantly optimises the healing process, accelerates the repair speed and improves the repair quality under simulated large-scale tendon injury conditions. The unique Janus surface design and the intelligent drug release function, in synergy, not only bring new hope to patients with large-scale tendon injuries, but also provide an important reference for the application of biomedical materials in the repair of complex tissues, which heralds the arrival of the era of more efficient and personalised tendon repair.

Bioinspired Asymmetric-Adhesion Janus Hydrogel Patch Regulating by Zwitterionic Polymers for Wet Tissues Adhesion and Postoperative Adhesion Prevention.

Asymmetrically adhesive hydrogel patch with robust wet tissue adhesion simultaneously anti-postoperative adhesion is essential for clinical applications in internal soft-tissue repair and postoperative anti-adhesion. Herein, inspired by the lubricative role of serosa and the underwater adhesion mechanism of mussels, an asymmetrically adhesive hydrogel Janus patch is developed with adhesion layer (AL) and anti-adhesion layer (anti-AL) through an in situ step-by-step polymerization process in the mold. The AL exhibits excellent adhesion to internal soft-tissues. In contrast, the anti-AL demonstrated ultralow fouling property against protein and fibroblasts, which hinders the early and advanced stages of development of the adhesion. Moreover, the Janus patch simultaneously promotes tissue regeneration via ROS clearance capability of catechol moieties in the AL. Results from in vivo experiments with rabbits and rats demonstrate that the AL strongly adheres to traumatized tissue, while the anti-AL surface demonstrate efficacy in preventing of post-abdominal surgery adhesions in contrast to clinical patches. Considering the advantages in terms of therapeutic efficacy and off the shelf, the Janus patch developed in this work presents a promise for preventing postoperative adhesions and promoting regeneration of internal tissue defects.

A Janus hydrogel that enables wet tissue adhesion and resists abdominal adhesions

Hydrogels have indeed achieved significant advancements, yet their clinical translation has been hampered by their inherent limitations in wet adhesion properties. Furthermore, the design of adhesive hydrogels that can resist postoperative adhesions remains an intricate challenge. In this study, we introduce a Janus hydrogel (JGP) that offers a novel approach to address these challenges. The JGP hydrogel has two asymmetrical sides, consisting of an adhesion layer (AL) and an anti-adhesion layer (AAL). Specifically, the AL incorporates three key components: N-[tris(hydroxymethyl)methyl]acrylamide (THMA), acrylic acid (AAc), and the acrylic acid N-hydroxysuccinimide ester (AAc-NHS). By drying the AL, it has a rapid water absorption capability. The abundance of hydroxyl and carboxyl groups in the AL enables the formation of robust hydrogen bonds with tissues, thereby achieving superior adhesive properties. Additionally, the synergistic effect of THMA's tridentate hydrogen bonding and the covalent bonding formed by AAc-NHS with tissue ensures long-lasting wet adhesion. To realize the anti-adhesion function, one side of the AL was immersed in a solution of [2-(methacryloyloxy)ethyl]dimethyl-(3-sulfopropyl)ammonium hydroxide (SBMA), which undergoes crosslinking to form the AAL. A comprehensive series of tests have confirmed that the JGP hydrogel exhibits exceptional mechanical properties, efficient and enduring adhesion, excellent biocompatibility, and degradability. Moreover, it possesses remarkable hemostatic properties and robust anti-abdominal adhesion characteristics.

Engineered Janus hydrogels: biomimetic surface engineering and biomedical applications.

Hydrogel bioadhesives, when applied to dysfunctional tissues substituting the epidermis or endothelium, exhibit compelling characteristics that enable revolutionary diagnostic and therapeutic procedures. Despite their demonstrated efficacy, these hydrogels as soft implants are still limited by improper symmetric surface functions, leading to postoperative complications and disorders. Janus hydrogel bioadhesives with unique asymmetric surface designs have thus been proposed as a reliable and biocompatible hydrogel interface, mimicking the structural characteristics of natural biological barriers. In this comprehensive review, we provide guidelines for the rational design of Janus hydrogel bioadhesives, covering methods for hydrogel surface chemistry and microstructure engineering. The engineering of Janus hydrogels is highlighted, specifically in tuning the basal surface to facilitate instant and robust hydrogel-tissue integration and modulating the apical surface as the anti-adhesion, anti-fouling, and anti-wear barrier. These asymmetric designs hold great potential in clinical translation, supporting applications including hemostasis/tissue sealing, chronic wound management, and regenerative medicine. By shedding light on the potential of Janus hydrogels as bioactive interfaces, this review paper aims to inspire further research and overcome current obstacles for advancing soft matter in next-generation healthcare.

A self-floating and windproof Janus biomass composite hydrogel with magnetic controllability and salt rejection for polluted seawater desalination

To alleviate the global freshwater crisis, a self-floating magnetic Janus biomass composite hydrogel has been fabricated through a rational asymmetric bilayer structure design, which exhibits many merits such as remarkable light-absorption, photothermal conversion, water-evaporation, salt rejection, wind-resistant, etc. Specifically, sodium alginate, cellulose nanofibrils (from corn straw), and acrylic acid were crosslinked by triple interpenetrating networks (chemical cross-linking, ionic cross-linking and hydrogen bonding). Janus hydrogel evaporator was constructed by incorporating the top layer containing light-absorbing core–shell magnetic nanoparticles (Fe3O4@PDA NPs), and the bottom layer composed of self-floating foam gel due to the addition of foaming agent. Under one solar irradiation, the average evaporation rate and photothermal conversion efficiency of Janus biomass composite hydrogel reached 2.89 ± 0.09 kg·m−2·h−1 and 95.66 ± 2.68 %, respectively. Its evaporation stability and salt tolerance capability have been demonstrated by extended period of simulated desalination. Furthermore, Janus biomass composite hydrogel also had excellent mechanical property (ultimate stress of 1.6 MPa) and magnetic performance, which can not only effectively resist the stress induced by wind and waves, but also enable the magnetic maneuvering and wind-resistance floating on the sea. When the input voltage of electromagnet was 24 V, the furtherest response displacement and maximum resisted wind speed were 9 cm and 7.2 m/s, respectively. Therefore, such magnetic self-floating Janus biomass composite hydrogel serving as interfacial solar-driven evaporator system offers a green, efficient and sustainable solution for clean freshwater production.

Janus hydrogel loaded with a CO2-generating chemical reaction system: Construction, characterization, and application in fruit and vegetable preservation

In this study, we inserted a dynamic chemical reaction system that can generate CO2 into Janus hydrogel (JH) to develop a multidimensional preservation platform that integrates hygroscopicity, antibacterial activity, and modified atmospheric capacity. The double gel system developed using sodium alginate/trehalose at a 1:1 ratio effectively encapsulated 90% of citric acid. Furthermore, CO2 loss was avoided by separately embedding NaHCO3/cinnamon essential oil and citric acid microcapsules into a gelatin pad to develop JH. Freeze-dried JH exhibited a porous and asymmetric structure, very strongly absorbing moisture, conducting water, and rapidly releasing CO2 and essential oils. Furthermore, when preserving various fruits and vegetables in practical settings, JH provided several preservation effects, including color protection, microbial inhibition, and antioxidant properties. Our study findings broaden the application of JH technology for developing chemical reaction systems, with the resulting JH holding substantial promise for cold chain logistics.

A Sprayable Janus Hydrogel as an Effective Bioadhesive for Gastrointestinal Perforation Repair

AbstractAdvancements in hydrogel bioadhesives for sealing gastrointestinal perforations (GP) face challenges due to weak mechanical properties, causing leakage, especially on uneven wound surfaces. Herein, a Janus hydrogel is introduced featuring a two‐step cross‐linking process, designed to serve as an efficient bioadhesive using a sprayable method. This Janus hydrogel formulation is achieved by modifying a photocurable hyaluronic acid hydrogel with dopamine (DA) and phenylboronic acid (PBA) groups, enabling reversible boronate ester bonds. These dynamic cross‐linking bonds facilitate shear‐thinning and self‐healing abilities, ensuring secure adhesion to complex wounds. A subsequent photocurable irreversible cross‐linking stage results in the formation of a hydrogel barrier with asymmetric adhesive properties, imparting inherent mechanical strength for postoperative anti‐adhesion. To enhance the clinical practicality of this hydrogel, an integrated sprayer device is further developed, enabling the efficient delivery of hydrogel at any angle and over long distances under minimally invasive conditions. Therefore, the HADP hydrogel, integrated with the sprayer device, successfully addressed the limitations associated with hydrogel bioadhesives in clinical applications concerning angles and terrains. This integrated approach presents a compelling solution for repairing gastrointestinal perforations in clinical settings. Moreover, it demonstrates significant potential for diverse applications in repairing complex wound surfaces.

A Tough Janus Hydrogel Patch with Strong Wet Adhesion and Self-Debonding for Oral Ulcer Treatment

A Tough Janus Hydrogel Patch with Strong Wet Adhesion and Self-Debonding for Oral Ulcer Treatment

A Single-Component Janus Zwitterionic Hydrogel Patch with a Bionic Microstructure for Postoperative Adhesion Prevention.

The development of anti-adhesion hydrogels for preventing postoperative adhesions is an ongoing challenge, particularly in achieving a balance between exceptional antifouling properties and effective in situ tissue retention. In this study, we propose a unique approach with the design of a single-component Janus zwitterionic hydrogel patch featuring a bionic microstructure. The Janus patches were prepared through free radical polymerization of sulfobetaine methacrylate with N, N'-methylenebis(2-propenamide) as the cross-linker. The incorporation of hexagonal facets separated by interconnecting grooves on one side imparts durable and reliable in situ retention capabilities to the Janus hydrogel patch when it is applied to traumatized tissues. The opposing flat surface exhibits outstanding resistance to bacteria, proteins, and cell adhesion, due to the superhydrophilicity and excellent antifouling characteristics of zwitterionic polymers. This dual functionality empowers the Janus hydrogel patch to mitigate adhesions between traumatized and surrounding tissues. The hexagonal and groove bionic microstructures facilitate rapid drainage, promoting swift contact with the tissue for increased adhesion strength, while independent hexagonal microfacets enhance the peeling energy. In an in vivo setting, Janus zwitterionic hydrogel patches with surface microstructures form mutually embedded structures with the cecum surface, minimizing the likelihood of slippage and detachment. Remarkably, in vivo experiments involving abdominal wall cecum injuries illustrate the Janus zwitterionic hydrogel patch's superior anti-adhesion effectiveness compared to commercial controls. Thus, the Janus hydrogel patch, distinguished by its bionic microstructure surface, presents substantial potential in the biomedical field for averting postoperative adhesions.

A multi-responsive actuator with sensing capability based on poly (N-isopropyl acrylamide)/poly (sodium acrylate) Janus hydrogels

A Janus hydrogel composed of temperature-responsive poly (N-isopropyl acrylamide) (PNIPAM) and pH-responsive poly (sodium acrylate) (PSA) was fabricated from inexpensive monomers using a facile synthesis route. The asymmetric swelling between PNIPAM and PSA in different media and at different temperatures makes the Janus hydrogels have a multi-stimuli response, meanwhile, the interpenetrating layer between PNIPAM and PSA indicated a good interfacial adhesion for easy transfer of internal stress and deformation. Thus, the Janus hydrogels exhibited excellent advantages in actuator/sensor engineering, demonstrating the potential to grip and release objects in toxic media, encrypt, monitor and control safety in chemical production, and alert temperature of flammable and explosive solvents. In addition, the features of the Janus hydrogels incorporated with carbon nanotubes, such as the high sensitivity, large stretchability, and rapid and linear response, enabled their application as strain sensors for wearable technologies in the recognition of body movement and health detection.

Implantable Resistive Strain Sensor-Decorated Colloidal Crystal Hydrogel Catheter for Intestinal Tract Pressure Sensing.

In the quest to develop advanced monitoring systems for intestinal peristaltic stress, this study introduces a groundbreaking approach inspired by nature's sensory networks. By the integration of novel materials and innovative manufacturing techniques, a multifunctional Janus hydrogel patch has been engineered. This unique patch not only demonstrates superior stress-sensing capabilities in the intricate intestinal environment but also enables adhesion to wet tissue surfaces. This achievement opens new avenues for real-time physiological monitoring and potential therapeutic interventions in the realm of gastrointestinal health.

Inside Cover Picture

Inspired by the skin of Osteichthyes fishes, a Janus hydrogel coating consisting of slippery and sticky layers is successfully prepared by a two‐step UV light irradiation at room temperature. The slippery layer replicates the structure of cycloid scales, while the nature of hydrogel mimics the mucus on fish skin. The Janus hydrogel coating possesses prominent mechanical, anti‐fouling and drag reduction properties. More details are discussed in the article by Xue et al. on page 867—872.image

Strong-adhesion and nonfouling self-generating zwitterionic Janus hydrogel paint

Zwitterionic hydrogel paints are promising and ecofriendly materials to prevent biofouling and oil contamination. However, the weak adhesion of hydrogel paints to substrates and tedious fabrication and coating processes limit their practical applications. Herein, a novel self-generating zwitterionic Janus hydrogel paint consisting of a polymer copolymerized by methyl methacrylate (MMA), tertiary carboxybetaine triisopropylsilyl ester ethyl acrylate (TCBSi), and 3-(methacryloxypropyl) trimethoxysilane (KH570) is reported. The polymer, when coated on a substrate, self-crosslinks into the polymer network and interlinks to the substrate during curing. This polymer decouples polymerization from the crosslinking and interlinking processes. When used underwater, the top layer of the coating rapidly hydrolyzes and self-generates a zwitterionic hydrogel layer, whereas the hydrophobic bottom layer remains unhydrolyzed. Adhesion tests show that this coating has considerably stronger adhesion strength than traditional zwitterionic hydrogel coatings due to the synergistic effect of hydrophobic interactions and interface bonding. Moreover, it has excellent resistance to protein, bacteria (Escherichia coli, Staphylococcus aureus, and Pseudomonas sp.), and diatom (Navicula incerta). The self-generating zwitterionic Janus hydrogel coating can also prevent oil contamination. This study serves as a promising avenue for the design and fabrication as well as practical application of self-generating zwitterionic Janus hydrogel paint with strong substrate adhesion.

Magneto-Induced Janus Adhesive-Tough Hydrogels for Wearable Human Motion Sensing and Enhanced Low-Grade Heat Harvesting.

Janus hydrogels with different properties on the two surfaces have considerable potential in the field of material engineering applications. Various Janus hydrogels have been developed, but there are still some problems, such as stress mismatch caused by the double-layer structure and Janus failure caused by material diffusion in the gradient structure. Here, we report a Janus adhesive-tough hydrogel with polydopamine-decorated Fe3O4 nanoparticles (Fe3O4@PDA) at one side induced by magnetic field to avoid uncontrollable material diffusion in the cross-linking polymerization of acrylamide with alginate-calcium. The magneto-induced Janus (MIJ) hydrogel has an adhesive surface and a tough bulk without an obvious interface to avoid stress mismatch. Due to the intrinsic dissipative matrix and the abundant catechol groups on the adhesive surface, it shows strong adhesion onto various substrates. The MIJ hydrogel has high sensitivity (GF = 0.842) in detecting tiny human motion. Owing to the synergy of Fe3O4@PDA-enhanced interfacial adhesion and heat transfer, it is possible to quickly generate effective temperature differences when adhering to human skin. The MIJ hydrogel achieves a Seebeck coefficient of 13.01 mV·K-1 and an output power of 462.02 mW·m-2 at a 20 K temperature difference. This work proposes a novel strategy to construct Janus hydrogels for flexible wearable devices in human motion sensing and low-grade heat harvesting.

Janus Hydrogel with Both Sticky Adhesion and Slippery Antifouling Properties for Strain Sensing

Janus Hydrogel with Both Sticky Adhesion and Slippery Antifouling Properties for Strain Sensing

Facile Bond Exchanging Strategy for Engineering Wet Adhesion and Antioxidant/Antibacterial Thin Layer over a Dynamic Hydrogel via the Carbon Dots Derived from Tannic Acid/ε-Polylysine.

Adhesive hydrogels, playing an essential role in stretchable electronics, soft robotics, tissue engineering, and so forth, upon functioning often need to adhere to various substrates in wet conditions and simultaneously exhibit antibacterial/antioxidant properties while possessing the intrinsic stretchability and elasticity of the hydrogel network intact. Therefore, simple approaches to conveniently access adhesive hydrogels with multifunctional surfaces are being pursued. Herein, a facile strategy has been proposed to construct multifunctional adhesive hydrogels via surface engineering of a multifunctional carbon dot (CD)-decorated polymeric thin layer by dynamic bond exchange. By this strategy, a double cross-linked network hydrogel of polyacrylamide (PAM) and oxidized dextran (ODA) was engineered with a unique dense layer over the Schiff base hydrogel matrix by aqueous solution immersion of PA-120, versatile CDs derived from tannic acid (TA) and ε-polylysine (PL). Without any additional agents, the PA-120 CDs with residual polyphenolic/catechol and amine moieties were incorporated into the surface structure of the hydrogel network by the combined action of the Schiff base and hydrogen bonds to form a dense surface layer that can exhibit high wet adhesive performance via the amine-polyphenol/catechol pair. The armor-like dense architecture also endowed hydrogels with considerably enhanced tensile/compression properties and excellent antioxidant/antibacterial abilities. Besides, the single-sided modified Janus hydrogel and completely surface-modified hydrogel can be flexibly developed through this approach. This strategy will provide new insights into the preparation and application of surface-modified hydrogels featuring multiple functions and tunable interfacial properties.