Zwitterion Functionalized Graphene Oxide/Polyacrylamide/Polyacrylic Acid Hydrogels with Photothermal Conversion and Antibacterial Properties for Highly Efficient Uranium Extraction from Seawater

In this study, graphene oxide (GO) and polyacrylamide/polyacrylic acid (PAM/PAA) are used to prepare hydrogels with photothermal conversion properties for highly efficient uranium extraction from seawater. Zwitterionic 2-methacryloyloxy ethyl phosphorylcholine (MPC) is introduced in the PAM/PAA/GO hydrogel to obtain PAM/PAA/GO/MPC (PAGM), exhibiting good antibacterial properties. PAGM demonstrates efficient and specific adsorption of uranium (VI) (U(VI)). Under light conditions, the adsorption capacity of PAGM reaches 196.12 mg g⁻¹ (pH = 8, t = 600 min, C₀ = 99.8 mg L⁻¹, m/v = 0.5 g L⁻¹). The adsorption capacity is only 160.29 mg g⁻¹ under dark conditions (pH = 8, t = 600 min, C₀ = 99.8 mg L⁻¹, m/v = 0.5 g L⁻¹). The adsorption capacity of light is 22.5% higher than that of dark. The adsorption process is fitted using the Langmuir and pseudo-second-order models. Furthermore, PAGM exhibits good repeatability and stability after five adsorption–desorption cycles. PAGM exhibits a U(VI) adsorption capacity of 6.1 mg g⁻¹ after storage for one month in natural seawater. The X-ray photoelectron spectroscopy (XPS) results demonstrate that the coordination of the amino, carboxyl, and hydroxyl groups with U(VI) is the primary mechanism of U(VI) adsorption. The mechanism is confirmed through detailed density functional theory calculations. PAGM demonstrates durability, high efficiency, photothermal conversion properties, and antibacterial properties. Thus, it is a promising candidate for uranium extraction from seawater.     

Rational Design of Porous Nanofiber Adsorbent by Blow‐Spinning with Ultrahigh Uranium Recovery Capacity from Seawater

Highly efficient recovery of uranium from seawater is of great concern because of the growing demand for nuclear energy. The use of amidoxime‐based polymeric fiber adsorbents is considered to be a promising approach because of their relatively high specificity and affinity to uranyl. The surface area, hydrophility, and surface charge of the adsorbent are reported to be critical factors that influence uranium recovery efficiency. Here, a porous amidoxime‐based nanofiber adsorbent (SMON–PAO) that exhibits the highest uranium recovery capacity among the existing fiber adsorbents both in 8 ppm uranium spiked seawater (1089.36 ± 64.31 mg‐U per g‐Ads) and in natural seawater (9.59 ± 0.64 mg‐U per g‐Ads) is prepared by blow spinning. These nanofibers are obtained by compositing polyacrylamidoxime with montmorillonite and exhibit the increased surface area and more exposed functional amidoxime moieties for uranyl adsorption. The residual montmorillonite enhances the hydrophility and reduces the negative surface charge, thereby increasing the contact of the adsorbent with seawater and reducing the charge repulsion between negative amidoxime group and negative uranyl species ([UO₂(CO₃)₃]^4?). The finding of this study indicates that rational design of uranium recovery adsorbents by comprehensive utilizing the key factors that influence uranium recovery performance is a promising approach for developing economically feasible uranium recovery materials.     

Photothermal-Enhanced Uranium Extraction from Seawater: A Biomass Solar Thermal Collector with 3D Ion-Transport Networks

Access to uranium resources is critical to the sustainable development of nuclear energy. The ocean contains abundant uranium resources, but the marine biological pollution and the low concentration of uranium make it a giant challenge to extract uranium from seawater. On the foundation of selective uranium adsorption using high uranium-affinity groups, realizing the external-field improved uranium capture without extra energy consumption is highly attractive. A solar thermal collector with 3D ion-transport networks based on environmentally friendly biomass adsorption material is reported, which contains antibacterial adsorption ligands and photothermal graphene oxide. The antibacterial ability through an easy one-step reaction and the fast mass transfer caused by photothermal conversion collaboratively improve the original adsorption capacity of the hydrogel by 46.7%, reaching 9.18 mg g⁻¹ after contact with natural seawater for 14 days. This study provides a universal strategy for the design of physical-fields-enhanced hydrogel adsorbents.     

Large Multipurpose Exceptionally Conductive Polymer Sponges Obtained by Efficient Wet‐Chemical Metallization

Exceptionally conductive (250 S cm^?1), very fast electrically heatable, thermally insulating, antimicrobial 3D polymeric sponges with very low density (≈30 mg cm^?3), superhydrophobicity, and high porosity, their method of preparation, and manifold examples for applications are presented here. The electrical heatability is reversible, reaching 90 °C with 4.4 W in about 19–20 s and cooling immediately on switching off the voltage. The sponges show high contact angles >150° against water on the sponge surface as well as inside the sponge. Water droplets injected into the sponges are ejected. A facile wet‐chemical method established for macroscopic melamine–formaldehyde sponges is the key for the thorough in‐depth surface metallization of the sponges. The coating thickness and uniformity depend on the metallization formulation, conditions of metallization, and the type of metal used. A scanning electron microscope is used for morphology characterization. A reduced metallization rate in air is highly critical for the in‐depth uniform coating of metals. The resulting metallized sponges could be highly interesting for heating as well as insulation devices in addition to oil/water separation membranes.     

Open-Cell Robust COF-Nanowire Network Sponges as Sustainable Adsorbent and Filter

Constructing crystalline covalent organic frameworks (COF) robust 3D reusable macroscopic objects exposing more adsorption sites with high water flux for use as a filter is an unresolved challenge. A simple scalable procedure is shown for making a robust, highly compressible 3D crystalline COF nanowire interconnected porous open-cell sponge. The compressive strength and Young's modulus (80% strain) of the sponge are 175 and 238 kPa, respectively. The sponge can withstand multiple compression-release cycles and a load of 2800 times its weight without collapsing. As an exemplary application, the use of a COF sponge in the selective removal and separation of cationic model dye from a mixture of dyes in water by adsorption and filtration with >99% efficiency is shown. Depending on the dye concentration, the dye removal time can be as short as 2 min, and dye adsorption efficiency can be as high as 653 mg g⁻¹ (COF in the sponge). During filtration, the sponges as filters show a high water flux of 2355 L h⁻¹ m⁻² under ambient conditions and maintain their performance for many cycles. The lightweight, reusability, and efficiency make present sponges sustainable materials as adsorbents and filters.     

Π-Skeleton Tailoring of Olefin-Linked Covalent Organic Frameworks Achieving Low Exciton Binding Energy for Photo-Enhanced Uranium Extraction from Seawater

Adsorption-photocatalysis technology based on covalent organic frameworks (COFs) offers an alternative method for advancing the field of uranium extraction from seawater. When determining the photocatalytic activity of COFs, the binding energy of excitons (E_b) functions is the decisive factor. Nevertheless, the majority of reported COFs have a large E_b, which seriously restricts their application in the field of photocatalysis. Using a practical π-skeleton engineering strategy, the current study synthesizes three donor-acceptor olefin-linked COFs containing amidoxime units in an effort to minimize E_b. Theoretical and experimental results reveal that the construction of planar and continuous π-electron delocalization channels can significantly reduce E_b and promote the separation of electron-hole pairs, thereby enhancing the photocatalytic activities. Moreover, the E_b of the TTh-COF-AO with a planar π-skeleton donor is significantly reduced, and exhibits a substantially smaller E_b (38.4 meV). Under visible light irradiation, a high photo-enhanced uranium extraction capacity of 10.24 mg g⁻¹ is achieved from natural seawater without the addition of sacrificial reagents, which is superior to the majority of olefin-linked COFs that have been reported to date. This study, therefore, paves the way for the development of tailored, efficient COFs photocatalysts for the extraction of uranium from seawater.     

Nanosized Copper Selenide Functionalized Zeolitic Imidazolate Framework‐8 (CuSe/ZIF‐8) for Efficient Immobilization of Gas‐Phase Elemental Mercury

A key challenge in elemental mercury (Hg⁰) decontamination from flue gas lies in the design of a sorbent with abundant reactive adsorption sites that exhibit high affinity toward Hg⁰ to simultaneously achieve rapid capture and large capacity. Herein, zeolitic imidazolate framework‐8 (ZIF‐8) supported copper selenide (CuSe) nanocomposites are synthesized by a newly designed two‐step surfactant‐assisted method. The as‐prepared CuSe/ZIF‐8 with CuSe to ZIF‐8 mass ratio of 80% (0.8NC‐ZIF) exhibits unparalleled performance toward Hg⁰ adsorption with equilibrium capacity and average rate reaching 309.8 mg g^?1 and 105.3 µg g^?1 min^?1, respectively, surpassing all reported metal sulfides and traditional activated‐carbon‐based sorbents. The impressive performance of 0.8NC‐ZIF for Hg⁰ immobilization is primarily attributed to the adequate exposure of the Se‐terminated sites with high affinity toward Hg⁰ resulted from the layered structure of CuSe. The adsorbed mercury selenide exhibits even higher stability than the most stable natural mercury ore—that is, mercury sulfide—hence minimizing its environmental impact when the CuSe/ZIF‐8 sorbent is dumped. This work provides a new mindset for future design of sorbents for efficient Hg⁰ capture from industrial flue gas. The results also justify the candidature of CuSe/ZIF to be applicable for mercury pollution remediation in real‐world conditions.     

Mussel‐Inspired Approach to Constructing Robust Multilayered Alginate Films for Antibacterial Applications

The exceptional mechanical properties of the byssus—the fibrous holdfast of mussels that provides underwater adhesion—have potential applications in medicine and technology. The catechol–Fe³⁺–catechol interaction underlies the unique properties of mussel byssus and has emerged as a tool for developing functional hybrid materials such as pH‐responsive, self‐healing gels. Herein, the construction of functional alginate (Alg) film on a solid substrate inspired by mussel byssus is reported. The approach consists of spin‐coating‐assisted deposition of Alg catechols onto a solid substrate and their subsequent crosslinking via catechol–Fe³⁺–catechol interactions. This yields robust and multilayered Alg films that are resistant to protein adsorption and suppress bacterial adhesion. This method can be used to create antibacterial films for coating implanted medical devices.     

3D Multiscale Superhydrophilic Sponges with Delicately Designed Pore Size for Ultrafast Oil/Water Separation

Developing novel filtering materials with both high permeation flux and rejection rate presents an enticing prospect for oil/water separation. In this paper, robust porous poly(melamine formaldehyde) (PMF) sponges with superwettability and controlled pore sizes through introducing layered double hydroxides (LDH) and SiO₂ electrospun nanofibers are reported. The LDH nanoscrolls endow the sponge with inherent superhydrophilicity and the SiO₂ nanofibers act as pore size regulators by overlapping the PMF mainframe. This approach allows the intrinsic large pores in the pristine sponge to decrease quickly from 109.50 to 23.35 µm, while maintaining porosity above 97.8%. The resulting modified sponges with varied pore sizes can effectively separate a wide range of oil/water mixtures, including the surfactant‐stabilized emulsions, solely by gravity, with ultrahigh permeation flux (maximum of 3 × 10⁵ L m^?2 h^?1 bar^?1) and satisfactory oil rejection (above 99.46%). Moreover, separation of emulsions stabilized by different surfactants, such as anionic, nonionic, and cationic surfactants has been investigated for further practical evaluation. It is expected that such a pore size tuning technology can provide a low cost and easily scaled‐up method to construct a series of filtering materials for high‐efficient separation of target oil/water mixtures.     

Facile Synthesis of Monodisperse Mesoporous Zirconium Titanium Oxide Microspheres with Varying Compositions and High Surface Areas for Heavy Metal Ion Sequestration

Monodisperse mesoporous zirconium titanium oxide microspheres with varying compositions (Zr content from 0 to 100%), high surface areas (up to 413 m²/g) and well‐interconnected mesopores are synthesized via a combined sol–gel self‐assembly and solvothermal process. Surface areas, pore diameters, crystallinity and mesostructures of the products are controlled by changing the composition of the microspheres. The resulting mesoporous microspheres are tested as adsorbents to remove Cr (VI) anions from solution and the binary oxides show very high adsorption capacities (>25.40 mg/g, that is 0.49 mmol/g) in contrast to previously reported oxides (4.25 mg/g for TiO₂, 4.47 mg/g for α‐Fe₂O₃, 5.8 mg/g for CeO₂). The maximum adsorption capacities of the mesoporous microspheres of varying compositions correlate with the amount of surface hydroxyl groups on the materials. A maximum adsorption capacity of 29.46 mg/g (0.57 mmol/g) is achieved on the microspheres containing 30% Zr due to abundant active hydroxyl groups for heavy metal ion adsorption. Owing to their integrated features (including variable compositions, high specific surface area, tunable pore size and monodisperse grain size) as well as specific acid‐base surface properties, such mesoporous zirconium titanium oxide microspheres are also expected to have potential either as catalysts or catalyst supports for industrial applications.     

3D Printing of Mechanically Stable Calcium‐Free Alginate‐Based Scaffolds with Tunable Surface Charge to Enable Cell Adhesion and Facile Biofunctionalization

For the 3D printing of bioscaffolds, the importance of a suitable bioink cannot be overemphasized. With excellent printability and biocompatibility, alginate (Alg) is one of the most used bioinks. However, its bioinert nature and insufficient mechanical stability, due to only crosslinking via cation interactions, hinder the practical application of Alg‐based bioinks in the individualized therapy of tissue defects. To overcome these drawbacks, for the first time, an ε‐polylysine (ε‐PL)‐modified Alg‐based bioink (Alg/ε‐PL) is produced. The introduction of ε‐PL improves the printability of the Alg‐based bioink due to increasing electrostatic interactions, which enhances the self‐supporting stability of the as‐printed scaffolds. The presence of the functional crosslinking –COOH and –NH₂ groups in Alg and ε‐PL under mild conditions further enhances the mechanical stability of the scaffolds, far exceeding that of Alg/Ca²⁺ scaffolds. The surface charge of the prepared scaffolds is finely tuned by the feed ratio of Alg to ε‐PL and postimmobilization of different quantities of additional ε‐PL, with a view to enhancing cell adhesion and further biofunctionalization. The results indicate that chondroitin sulfate, an extracellular matrix component, and vascular endothelial growth factor can be successfully applied to biofunctionalize the scaffolds via electrostatic adsorption for enhanced biological activity.     

A Nanoselenium Sponge for Instantaneous Mercury Removal to Undetectable Levels

Selective removal of aqueous mercury to levels below 10 ng L^?1 or part per trillion remains an elusive goal for public health and environmental agencies. Here, it is shown that a low‐cost nanocomposite sponge prepared by growing selenium (Se) nanomaterials on the surface and throughout the bulk of a polyurethane sponge exhibits a record breaking‐mercury ion (Hg²⁺) removal rate, regardless of the pH. The exposure of aqueous solutions containing 10 mg L^?1–12 ng L^?1 Hg²⁺ to the sponge for a few seconds results in clean water with undetectable mercury levels (detection limit: 0.2 ng L^?1). Such performance is far below the acceptable limits in drinking water (2 µg L^?1), industrial effluents (0.2 µg L^?1), and the most stringent surface water quality standards (1.3 ng L^?1). The sponge shows a unique preference for Hg, does not retain water nutrients, and can significantly reduce the concentration of other heavy metal pollutants. Furthermore, the sponge shows no cytotoxic effect on human cells while exhibiting strong antimicrobial properties. The high affinity of Hg for Se results in irreversible sequestration and detoxification of mercury by the sponge, confirming the suitability for landfill disposal.     

A Controllable Self‐Assembly Method for Large‐Scale Synthesis of Graphene Sponges and Free‐Standing Graphene Films

A simple method to prepare large‐scale graphene sponges and free‐standing graphene films using a speed vacuum concentrator is presented. During the centrifugal evaporation process, the graphene oxide (GO) sheets in the aqueous suspension are assembled to generate network‐linked GO sponges or a series of multilayer GO films, depending on the temperature of a centrifugal vacuum chamber. While sponge‐like bulk GO materials (GO sponges) are produced at 40 °C, uniform free‐standing GO films of size up to 9 cm² are generated at 80 °C. The thickness of GO films can be controlled from 200 nm to 1 µm based on the concentration of the GO colloidal suspension and evaporation temperature. The synthesized GO films exhibit excellent transparency, typical fluorescent emission signal, and high flexibility with a smooth surface and condensed density. Reduced GO sponges and films with less than 5 wt% oxygen are produced through a thermal annealing process at 800 °C with H₂/Ar flow. The structural flexibility of the reduced GO sponges, which have a highly porous, interconnected, 3D network, as well as excellent electrochemical properties of the reduced GO film with respect to electrode kinetics for the [Fe(CN)₆]^3?/4? redox system, are demonstrated.     

Seaweed‐Derived Electrospun Nanofibrous Membranes for Ultrahigh Protein Adsorption

Construction of simple and efficient protein adsorption materials is extremely vital to satisfy the requirements of highly purified proteins in biopharmaceutical and biotechnological industries, yet remains challenging. Herein, a cost‐effective strategy to develop seaweed‐derived nanofibrous membranes (NFM) for ultrahigh protein adsorption is reported. Synergistic regulation by cosolvent of ethanol, nonionic surfactants of Triton X‐100, and polyethylene oxide (PEO_5000k) is employed to realize electrospinning of seaweed‐derived sodium alginate (SA) nanofibers with higher alginate content of 98 wt% to date, and following water washing easily generates SA nanofibrous membranes (SA‐NFM) with excellent morphology. Benefiting from the nanoscale merit of large specific surface area and tortuously porous microstructure, SA‐NFM exhibit a high actual capacity of 1235 mg g^?1 toward lysozyme, which far exceeds maximum value for the reported 2D membrane materials (710 mg g^?1) and is about 20 times that of commercial membranes adsorbents (51 mg g^?1). Higher dynamic capacity of 805 mg g^?1 (gravity driven) is also realized to meet the demand of practical application. The SA‐NFM also possess outstanding reversibility and unique selectivity toward specific proteins. Herein, SA‐NFM represent a perfect candidate for next‐generation protein absorbents for fast and efficient bioseparation.     

Sponge‐Templated Preparation of High Surface Area Graphene with Ultrahigh Capacitive Deionization Performance

Capacitive deionization (CDI) is a competent water desalination technique offering an appropriate route to obtain clean water. However, a rational designed structure of the electrode materials is essentially required for achieving high CDI performance. Here, a novel sponge‐templated strategy is developed for the first time to prepare graphene sheets with high specific surface area and suitable pore size distribution. Sponge is used as the support of graphene oxide to prevent the restack of graphene sheets, as well as to suppress the agglomerate during the annealing process. Importantly, the as‐fabricated graphene sheets possess high specific surface area of 305 m² g^?1 and wide pore size distribution. Ultrahigh CDI performance, a remarkable electrosorptive capacity of 4.95 mg g^?1, and siginificant desorption rate of 25 min, is achieved with the sponge‐templated prepared graphene electrodes. This work provides an effective solution for the synthesis of rational graphene architectures for general applications in CDI, energy storage and conversion.     

Few‐Layered SnS2 on Few‐Layered Reduced Graphene Oxide as Na‐Ion Battery Anode with Ultralong Cycle Life and Superior Rate Capability

Na‐ion Batteries have been considered as promising alternatives to Li‐ion batteries due to the natural abundance of sodium resources. Searching for high‐performance anode materials currently becomes a hot topic and also a great challenge for developing Na‐ion batteries. In this work, a novel hybrid anode is synthesized consisting of ultrafine, few‐layered SnS₂ anchored on few‐layered reduced graphene oxide (rGO) by a facile solvothermal route. The SnS₂/rGO hybrid exhibits a high capacity, ultralong cycle life, and superior rate capability. The hybrid can deliver a high charge capacity of 649 mAh g^?1 at 100 mA g^?1. At 800 mA g^?1 (1.8 C), it can yield an initial charge capacity of 469 mAh g^?1, which can be maintained at 89% and 61%, respectively, after 400 and 1000 cycles. The hybrid can also sustain a current density up to 12.8 A g^?1 (≈28 C) where the charge process can be completed in only 1.3 min while still delivering a charge capacity of 337 mAh g^?1. The fast and stable Na‐storage ability of SnS₂/rGO makes it a promising anode for Na‐ion batteries.     

Smart Photonic Crystal Hydrogel Material for Uranyl Ion Monitoring and Removal in Water

Uranyl ion (UO₂²⁺) pollution is a serious environmental problem, and developing novel adsorption materials is essential for UO₂²⁺ monitoring and removal. Although some progress is achieved, it is still a challenging task to develop an adsorption material with indicating signal for real‐time evaluation of the adsorption degree and the UO₂²⁺ concentration. Herein, this paper describes a smart photonic crystal hydrogel (PCH) material, which not only can be used for real‐time monitoring function but also can be utilized for UO₂²⁺ removal based on the chelation of UO₂²⁺ with ligand groups in PCH material. The working principle is based on the binding of a uranyl ion to multiple ligand groups, which results in the shrinkage of PCH material and triggers a blue‐shift of diffraction wavelength. Consequently, the adsorption degree and the UO₂²⁺ concentration can be sensitively evaluated by measuring the diffraction shift or observing the color change with naked eye. With this PCH material, the lowest detectable concentration for UO₂²⁺ is 10 × 10^?9m , and the maximum adsorption capacity at 298 K is 169.67 mmol kg^?1. In addition, this material also holds good selectivity and regeneration feature, and shows desirable performance for UO₂²⁺ analysis in real water samples.     

Highly Stretchable,Elastic, and Ionic Conductive Hydrogel for Artificial Soft Electronics

High conductivity, large mechanical strength, and elongation are important parameters for soft electronic applications. However, it is difficult to find a material with balanced electronic and mechanical performance. Here, a simple method is developed to introduce ion‐rich pores into strong hydrogel matrix and fabricate a novel ionic conductive hydrogel with a high level of electronic and mechanical properties. The proposed ionic conductive hydrogel is achieved by physically cross‐linking the tough biocompatible polyvinyl alcohol (PVA) gel as the matrix and embedding hydroxypropyl cellulose (HPC) biopolymer fibers inside matrix followed by salt solution soaking. The wrinkle and dense structure induced by salting in PVA matrix provides large stress (1.3 MPa) and strain (975%). The well‐distributed porous structure as well as ion migration–facilitated ion‐rich environment generated by embedded HPC fibers dramatically enhances ionic conductivity (up to 3.4 S m^?1, at f = 1 MHz). The conductive hybrid hydrogel can work as an artificial nerve in a 3D printed robotic hand, allowing passing of stable and tunable electrical signals and full recovery under robotic hand finger movements. This natural rubber‐like ionic conductive hydrogel has a promising application in artificial flexible electronics.     

Biomimetic Thermo-Sensitive Hydrogel Encapsulating Hemangiomas Stem Cell Derived Extracellular Vesicles Promotes Microcirculation Reconstruction in Diabetic Wounds

Tissue repair and regeneration in ischemic areas require effective strategies for angiogenesis and microcirculation reconstruction. In this research, extracellular vesicles (EVs) derived from hemangioma stem cells (HemSC) are used as bio-functional materials for angiogenesis. In addition, a novel thermo-sensitive hydrogel based on chitosan (CS) and modified with hyaluronic oligosaccharides (oHA), is specially developed as an ideal carrier of HemSC-EVs. The oHA/CS^gel provides a sustained-release delivery system for EVs, enhances the angiogenic function of HemSC-EVs, and exerts other bio-functions to comprehensively accelerate tissue repair. The physical properties of EVs@oHA/CS^gel proved to be soft, highly elastic deformable, biocompatible, and can maintain the shape and structure of EVs. In vitro co-culture assay verifies the angiogenic effect of EVs@oHA/CS^gel, and this effect is also evaluated in a diabetic wound model. Compared to untreated group, the EVs@oHA/CS^gel group has only 26.9% wound area on day 14, and 226.8% blood flux mark on day 17. Pharmacological mechanisms of HemSC-EVs are predicted by RNA-seq, and cluster analysis of miRNAs predicted targets presents several up-regulated biological processes involving in angiogenesis and wound healing. In conclusion, it is suggested that EVs@oHA/CS^gel as a satisfying therapeutic system for microcirculation reconstruction in tissue repair.     

Conductive “Smart” Hybrid Hydrogels with PNIPAM and Nanostructured Conductive Polymers

Stimuli‐responsive hydrogels with decent electrical properties are a promising class of polymeric materials for a range of technological applications, such as electrical, electrochemical, and biomedical devices. In this paper, thermally responsive and conductive hybrid hydrogels are synthesized by in situ formation of continuous network of conductive polymer hydrogels crosslinked by phytic acid in poly(N‐isopropylacrylamide) matrix. The interpenetrating binary network structure provides the hybrid hydrogels with continuous transporting path for electrons, highly porous microstructure, strong interactions between two hydrogel networks, thus endowing the hybrid hydrogels with a unique combination of high electrical conductivity (up to 0.8 S m^?1), high thermoresponsive sensitivity (significant volume change within several seconds), and greatly enhanced mechanical properties. This work demonstrates that the architecture of the filling phase in the hydrogel matrix and design of hybrid hydrogel structure play an important role in determining the performance of the resulting hybrid material. The attractive performance of these hybrid hydrogels is further demonstrated by the developed switcher device which suggests potential applications in stimuli‐responsive electronic devices.