Enhanced Photocarrier Generation with Selectable Wavelengths by M‐Decorated‐CuInS2 Nanocrystals (M = Au and Pt) Synthesized in a Single Surfactant Process on MoS2 Bilayers

A facile approach for the synthesis of Au‐ and Pt‐decorated CuInS₂ nanocrystals (CIS NCs) as sensitizer materials on the top of MoS₂ bilayers is demonstrated. A single surfactant (oleylamine) is used to prepare such heterostructured noble metal decorated CIS NCs from the pristine CIS. Such a feasible way to synthesize heterostructured noble metal decorated CIS NCs from the single surfactant can stimulate the development of the functionalized heterostructured NCs in large scale for practical applications such as solar cells and photodetectors. Photodetectors based on MoS₂ bilayers with the synthesized nanocrystals display enhanced photocurrent, almost 20–40 times higher responsivity and the On/Off ratio is enlarged one order of magnitude compared with the pristine MoS₂ bilayers‐based photodetectors. Remarkably, by using Pt‐ or Au‐decorated CIS NCs, the photocurrent enhancement of MoS₂ photodetectors can be tuned between blue (405 nm) to green (532 nm). The strategy described here acts as a perspective to significantly improve the performance of MoS₂‐based photodetectors with the controllable absorption wavelengths in the visible light range, showing the feasibility of the possible color detection.     

Solution‐Processed 3D RGO–MoS2/Pyramid Si Heterojunction for Ultrahigh Detectivity and Ultra‐Broadband Photodetection

Molybdenum disulfide (MoS₂), a typical 2D metal dichalcogenide (2DMD), has exhibited tremendous potential in optoelectronic device applications, especially in photodetection. However, due to the weak light absorption of planar mono‐/multilayers, limited cutoff wavelength edge, and lack of high‐quality junctions, most reported MoS₂‐based photodetectors show undesirable performance. Here, a structurized 3D heterojunction of RGO–MoS₂/pyramid Si is demonstrated via a simple solution‐processing method. Owing to the improved light absorption by the pyramid structure, the narrowed bandgap of the MoS₂ by the imperfect crystallinity, and the enhanced charge separation/transportation by the inserted reduced graphene oxide (RGO), the assembled photodetector exhibits excellent performance in terms of a large responsivity of 21.8 A W^?1, extremely high detectivity up to 3.8 × 10¹⁵ Jones (Jones = cm Hz^1/2 W^?1) and ultrabroad spectrum response ranging from 350 nm (ultraviolet) to 4.3 µm (midwave infrared). These device parameters represent the best results for MoS₂‐based self‐driven photodetectors, and the detectivity value sets a new record for the 2DMD‐based photodetectors reported thus far. Prospectively, the design of novel 3D heterojunction can be extended to other 2DMDs, opening up the opportunities for a host of high‐performance optoelectronic devices.     

Nanoparticle‐Enhanced Silver‐Nanowire Plasmonic Electrodes for High‐Performance Organic Optoelectronic Devices

Improved performance in plasmonic organic solar cells (OSCs) and organic light‐emitting diodes (OLEDs) via strong plasmon‐coupling effects generated by aligned silver nanowire (AgNW) transparent electrodes decorated with core–shell silver–silica nanoparticles (Ag@SiO₂NPs) is demonstrated. NP‐enhanced plasmonic AgNW (Ag@SiO₂NP–AgNW) electrodes enable substantially enhanced radiative emission and light absorption efficiency due to strong hybridized plasmon coupling between localized surface plasmons (LSPs) and propagating surface plasmon polaritons (SPPs) modes, which leads to improved device performance in organic optoelectronic devices (OODs). The discrete dipole approximation (DDA) calculation of the electric field verifies a strongly enhanced plasmon‐coupling effect caused by decorating core–shell Ag@SiO₂NPs onto the AgNWs. Notably, an electroluminescence efficiency of 25.33 cd A^?1 (at 3.2 V) and a power efficiency of 25.14 lm W^?1 (3.0 V) in OLEDs, as well as a power conversion efficiency (PCE) value of 9.19% in OSCs are achieved using hybrid Ag@SiO₂NP–AgNW films. These are the highest values reported to date for optoelectronic devices based on AgNW electrodes. This work provides a new design platform to fabricate high‐performance OODs, which can be further explored in various plasmonic and optoelectronic devices.     

Atomic Cobalt Covalently Engineered Interlayers for Superior Lithium‐Ion Storage

With the unique‐layered structure, MXenes show potential as electrodes in energy‐storage devices including lithium‐ion (Li⁺) capacitors and batteries. However, the low Li⁺‐storage capacity hinders the application of MXenes in place of commercial carbon materials. Here, the vanadium carbide (V₂C) MXene with engineered interlayer spacing for desirable storage capacity is demonstrated. The interlayer distance of pristine V₂C MXene is controllably tuned to 0.735 nm resulting in improved Li‐ion capacity of 686.7 mA h g^?1 at 0.1 A g^?1, the best MXene‐based Li⁺‐storage capacity reported so far. Further, cobalt ions are stably intercalated into the interlayer of V₂C MXene to form a new interlayer‐expanded structure via strong V–O–Co bonding. The intercalated V₂C MXene electrodes not only exhibit superior capacity up to 1117.3 mA h g^?1 at 0.1 A g^?1, but also deliver a significantly ultralong cycling stability over 15 000 cycles. These results clearly suggest that MXene materials with an engineered interlayer distance will be a rational route for realizing them as superstable and high‐performance Li⁺ capacitor electrodes.     

Phase‐Engineered Type‐II Multimetal–Selenide Heterostructures toward Low‐Power Consumption,Flexible, Transparent,and Wide‐Spectrum Photoresponse Photodetectors

Phase‐engineered type‐II metal–selenide heterostructures are demonstrated by directly selenizing indium‐tin oxide to form multimetal selenides in a single step. The utilization of a plasma system to assist the selenization facilitates a low‐temperature process, which results in large‐area films with high uniformity. Compared to single‐metal–selenide‐based photodetectors, the multimetal–selenide photodetectors exhibit obviously improved performance, which can be attributed to the Schottky contact at the interface for tuning the carrier transport, as well as the type‐II heterostructure that is beneficial for the separation of the electron–hole pairs. The multimetal–selenide photodetectors exhibit a response to light over a broad spectrum from UV to visible light with a high responsivity of 0.8 A W^?1 and an on/off current ratio of up to 10². Interestingly, all‐transparent photodetectors are successfully produced in this work. Moreover, the possibility of fabricating devices on flexible substrates is also demonstrated with sustainable performance, high strain tolerance, and high durability during bending tests.     

High‐Responsivity Photodetection by a Self‐Catalyzed Phase‐Pure p‐GaAs Nanowire

Defects are detrimental for optoelectronics devices, such as stacking faults can form carrier‐transportation barriers, and foreign impurities (Au) with deep‐energy levels can form carrier traps and nonradiative recombination centers. Here, self‐catalyzed p‐type GaAs nanowires (NWs) with a pure zinc blende (ZB) structure are first developed, and then a photodetector made from these NWs is fabricated. Due to the absence of stacking faults and suppression of large amount of defects with deep energy levels, the photodetector exhibits room‐temperature high photoresponsivity of 1.45 × 10⁵ A W^?1 and excellent specific detectivity (D*) up to 1.48 × 10¹⁴ Jones for a low‐intensity light signal of wavelength 632.8 nm, which outperforms previously reported NW‐based photodetectors. These results demonstrate these self‐catalyzed pure‐ZB GaAs NWs to be promising candidates for optoelectronics applications.     

A Solid‐State Fibriform Supercapacitor Boosted by Host–Guest Hybridization between the Carbon Nanotube Scaffold and MXene Nanosheets

Fiber‐shaped supercapacitors with improved specific capacitance and high rate capability are a promising candidate as power supply for smart textiles. However, the synergistic interaction between conductive filaments and active nanomaterials remains a crucial challenge, especially when hydrothermal or electrochemical deposition is used to produce a core (fiber)–shell (active materials) fibrous structure. On the other hand, although 2D pseudocapacitive materials, e.g., Ti₃C₂T _x (MXene), have demonstrated high volumetric capacitance, high electrical conductivity, and hydrophilic characteristics, MXene‐based electrodes normally suffer from poor rate capability owing to the sheet restacking especially when the loading level is high and solid‐state gel is used as electrolyte. Herein, by hosting MXene nanosheets (Ti₃C₂T _x ) in the corridor of a scrolled carbon nanotube (CNT) scaffold, a MXene/CNT fiber with helical structure is successfully fabricated. These features offer open spaces for rapid ion diffusion and guarantee fast electron transport. The solid‐state supercapacitor based on such hybrid fibers with gel electrolyte coating exhibits a volumetric capacitance of 22.7 F cm⁻³ at 0.1 A cm⁻³ with capacitance retention of 84% at current density of 1.0 A cm⁻³ (19.1 F cm⁻³), improved volumetric energy density of 2.55 mWh cm⁻³ at the power density of 45.9 mW cm⁻³, and excellent mechanical robustness.     

Facet‐Dependent Optical Properties Revealed through Investigation of Polyhedral Au–Cu2O and Bimetallic Core–Shell Nanocrystals

The ability to prepare Au–Cu₂O core–shell nanocrystals with precise control over particle size and shape has led to the discovery of facet‐dependent optical properties in cuprous oxide crystals. The use of Au cores not only allows the successful formation of Au–Cu₂O core–shell nanocrystals with tunable sizes, but also enables the observation of facet‐dependent optical properties in these crystals through the Au localized surface plasmon resonance (LSPR) absorption band. By tuning the Cu₂O shell morphology from rhombic dodecahedral to octahedral and cubic structures, and thus the exposed facets, the Au LSPR band position can be widely tuned. Such facet‐dependent optical effects are not observed in bimetallic Au–Ag and Au–Pd core–shell nanocrystals with the same precisely tuned particle sizes and shapes. It is believed that similar facet‐dependent optical properties could be observed in other ionic solids and other metal–metal oxide systems. The unusually large degree of plasmonic band tuning covering from the visible to the near‐infrared region in this type of nanostructure should be quite useful for a range of plasmonic applications.     

Gate‐Controlled Graphene–Silicon Schottky Junction Photodetector

Various photodetectors showing extremely high photoresponsivity have been frequently reported, but many of these photodetectors could not avoid the simultaneous amplification of dark current. A gate‐controlled graphene–silicon Schottky junction photodetector that exhibits a high on/off photoswitching ratio (≈10⁴), a very high photoresponsivity (≈70 A W⁻¹), and a low dark current in the order of µA cm⁻² in a wide wavelength range (395–850 nm) is demonstrated. The photoresponsivity is ≈100 times higher than that of existing commercial photodetectors, and 7000 times higher than that of graphene‐field‐effect transistor‐based photodetectors, while the dark current is similar to or lower than that of commercial photodetectors. This result can be explained by a unique gain mechanism originating from the difference in carrier transport characteristics of silicon and graphene.     

Metal‐Halide Perovskites for Gate Dielectrics in Field‐Effect Transistors and Photodetectors Enabled by PMMA Lift‐Off Process

Metal‐halide perovskites have emerged as promising materials for optoelectronics applications, such as photovoltaics, light‐emitting diodes, and photodetectors due to their excellent photoconversion efficiencies. However, their instability in aqueous solutions and most organic solvents has complicated their micropatterning procedures, which are needed for dense device integration, for example, in displays or cameras. In this work, a lift‐off process based on poly(methyl methacrylate) and deep ultraviolet lithography on flexible plastic foils is presented. This technique comprises simultaneous patterning of the metal‐halide perovskite with a top electrode, which results in microscale vertical device architectures with high spatial resolution and alignment properties. Hence, thin‐film transistors (TFTs) with methyl‐ammonium lead iodide (MAPbI₃) gate dielectrics are demonstrated for the first time. The giant dielectric constant of MAPbI₃ (>1000) leads to excellent low‐voltage TFT switching capabilities with subthreshold swings ≈80 mV decade^?1 over ≈5 orders of drain current magnitude. Furthermore, vertically stacked low‐power Au‐MAPbI₃‐Au photodetectors with close‐to‐ideal linear response (R² = 0.9997) are created. The mechanical stability down to a tensile radius of 6 mm is demonstrated for the TFTs and photodetectors, simultaneously realized on the same flexible plastic substrate. These results open the way for flexible low‐power integrated (opto‐)electronic systems based on metal‐halide perovskites.     

Self‐Formed Channel Devices Based on Vertically Grown 2D Materials with Large‐Surface‐Area and Their Potential for Chemical Sensor Applications

2D layered materials with sensitive surfaces are promising materials for use in chemical sensing devices, owing to their extremely large surface‐to‐volume ratios. However, most chemical sensors based on 2D materials are used in the form of laterally defined active channels, in which the active area is limited to the actual device dimensions. Therefore, a novel approach for fabricating self‐formed active‐channel devices is proposed based on 2D semiconductor materials with very large surface areas, and their potential gas sensing ability is examined. First, the vertical growth phenomenon of SnS₂ nanocrystals is investigated with large surface area via metal‐assisted growth using prepatterned metal electrodes, and then self‐formed active‐channel devices are suggested without additional pattering through the selective synthesis of SnS₂ nanosheets on prepatterned metal electrodes. The self‐formed active‐channel device exhibits extremely high response values (>2000% at 10 ppm) for NO₂ along with excellent NO₂ selectivity. Moreover, the NO₂ gas response of the gas sensing device with vertically self‐formed SnS₂ nanosheets is more than two orders of magnitude higher than that of a similar exfoliated SnS₂‐based device. These results indicate that the facile device fabrication method would be applicable to various systems in which surface area plays an important role.     

Symmetry‐Reduction Enhanced Polarization‐Sensitive Photodetection in Core–Shell SbI3/Sb2O3 van der Waals Heterostructure

Structural symmetry is a simple way to quantify the anisotropic properties of materials toward unique device applications including anisotropic transportation and polarization‐sensitive photodetection. The enhancement of anisotropy can be achieved by artificial symmetry‐reduction design. A core–shell SbI₃/Sb₂O₃ nanowire, a heterostructure bonded by van der Waals forces, is introduced as an example of enhancing the performance of polarization‐sensitive photodetectors via symmetry reduction. The structural, vibrational, and optical anisotropies of such core–shell nanostructures are systematically investigated. It is found that the anisotropic absorbance of a core–shell nanowire is obviously higher than that of two single compounds from both theoretical and experimental investigations. Anisotropic photocurrents of the polarization‐sensitive photodetectors based on these core–shell SbI₃/Sb₂O₃ van der Waals nanowires are measured ranging from ultraviolet (UV) to visible light (360–532 nm). Compared with other van der Waals 1D materials, low anisotropy ratio (I_max/I_min) is measured based on SbI₃ but a device based on this core–shell nanowire possesses a relatively high anisotropy ratio of ≈3.14 under 450 nm polarized light. This work shows that the low‐symmetrical core–shell van der Waals heterostructure has large potential to be applied in wide range polarization‐sensitive photodetectors.     

Non‐Volatile ReRAM Devices Based on Self‐Assembled Multilayers of Modified Graphene Oxide 2D Nanosheets

2D nanomaterials have been actively utilized in non‐volatile resistive switching random access memory (ReRAM) devices due to their high flexibility, 3D‐stacking capability, simple structure, transparency, easy fabrication, and low cost. Herein, it demonstrates re‐writable, bistable, transparent, and flexible solution‐processed crossbar ReRAM devices utilizing graphene oxide (GO) based multilayers as active dielectric layers. The devices employ single‐ or multi‐component‐based multilayers composed of positively charged GO (N‐GO(+) or NS‐GO(+)) with/without negatively charged GO(‐) using layer‐by‐layer assembly method, sandwiched between Al bottom and Au top electrodes. The device based on the multi‐component active layer Au/[N‐GO(+)/GO(‐)]_n/Al/PES shows higher ON/OFF ratio of ≈10⁵ with switching voltage of ?1.9 V and higher retention stability (≈10⁴ s), whereas the device based on single component (Au/[N‐GO(+)]_n/Al/PES) shows ≈10³ ON/OFF ratio at ±3.5 V switching voltage. The superior ReRAM properties of the multi‐component‐based device are attributed to a higher coating surface roughness. The Au/[N‐GO(+)/GO(–)]_n/Al/PES device prepared from lower GO concentration (0.01%) exhibits higher ON/OFF ratio (≈10⁹) at switching voltage of ±2.0 V. However, better stability is achieved by increasing the concentration from 0.01% to 0.05% of all GO‐based solutions. It is found that the devices containing MnO₂ in the dielectric layer do not improve the ReRAM performance.     

A General Method for the Chemical Synthesis of Large‐Scale,Seamless Transition Metal Dichalcogenide Electronics

The capability to directly build atomically thin transition metal dichalcogenide (TMD) devices by chemical synthesis offers important opportunities to achieve large‐scale electronics and optoelectronics with seamless interfaces. Here, a general approach for the chemical synthesis of a variety of TMD (e.g., MoS₂, WS₂, and MoSe₂) device arrays over large areas is reported. During chemical vapor deposition, semiconducting TMD channels and metallic TMD/carbon nanotube (CNT) hybrid electrodes are simultaneously formed on CNT‐patterned substrate, and then coalesce into seamless devices. Chemically synthesized TMD devices exhibit attractive electrical and mechanical properties. It is demonstrated that chemically synthesized MoS₂–MoS₂/CNT devices have Ohmic contacts between MoS₂/CNT hybrid electrodes and MoS₂ channels. In addition, MoS₂–MoS₂/CNT devices show greatly enhanced mechanical stability and photoresponsivity compared with conventional gold‐contacted devices, which makes them suitable for flexible optoelectronics. Accordingly, a highly flexible pixel array based on chemically synthesized MoS₂–MoS₂/CNT photodetectors is applied for image sensing.     

High Detectivity Solar‐Blind High‐Temperature Deep‐Ultraviolet Photodetector Based on Multi‐Layered (l00) Facet‐Oriented β‐Ga2O3 Nanobelts

Fabrication of a high‐temperature deep‐ultraviolet photodetector working in the solar‐blind spectrum range (190–280 nm) is a challenge due to the degradation in the dark current and photoresponse properties. Herein, β‐Ga₂O₃ multi‐layered nanobelts with (l00) facet‐oriented were synthesized, and were demonstrated for the first time to possess excellent mechanical, electrical properties and stability at a high temperature inside a TEM studies. As‐fabricated DUV solar‐blind photodetectors using (l00) facet‐oriented β‐Ga₂O₃ multi‐layered nanobelts demonstrated enhanced photodetective performances, that is, high sensitivity, high signal‐to‐noise ratio, high spectral selectivity, high speed, and high stability, importantly, at a temperature as high as 433 K, which are comparable to other reported semiconducting nanomaterial photodetectors. In particular, the characteristics of the photoresponsivity of the β‐Ga₂O₃ nanobelt devices include a high photoexcited current (>21 nA), an ultralow dark current (below the detection limit of 10^?14 A), a fast time response (<0.3 s), a high R_λ (≈851 A/W), and a high EQE (～4.2 × 10³). The present fabricated facet‐oriented β‐Ga₂O₃ multi‐layered nanobelt based devices will find practical applications in photodetectors or optical switches for high‐temperature environment.     

Reverse‐Offset Printed Ultrathin Ag Mesh for Robust Conformal Transparent Electrodes for High‐Performance Organic Photovoltaics

Mechanically durable transparent electrodes are needed in flexible optoelectronic devices to realize their long‐term stable functioning, for applications in various fields such as energy, healthcare, and soft robotics. Several promising transparent electrodes based on nanomaterials have been previously reported to replace the conventional and fragile indium‐tin oxide (ITO); however, obtaining feasible printed transparent electrodes for ultraflexible devices with a multistack structure is still a great challenge. Here, a printed ultrathin (uniform thickness of 100 nm) Ag mesh transparent electrode is demonstrated, simultaneously achieving high conductance, high transparency, and good mechanical properties. It shows a 17 Ω sq^?1 sheet resistance (R_sh) with 93.2% transmittance, which surpasses the performance of sputtered ITO electrodes and other ultrathin Ag mesh transparent electrodes. The conductance is stable after 500 cycles of 100% stretch/release deformation, with an insignificant increase (10.6%) in R_sh by adopting a buckling structure. Furthermore, organic photovoltaics (OPVs) using our Ag mesh transparent electrodes achieve a power conversion efficiency of 8.3%, which is comparable to the performance of ITO‐based OPVs.     

Direct Laser‐Patterned Micro‐Supercapacitors from Paintable MoS2 Films

Micrometer‐sized electrochemical capacitors have recently attracted attention due to their possible applications in micro‐electronic devices. Here, a new approach to large‐scale fabrication of high‐capacitance, two‐dimensional MoS₂ film‐based micro‐supercapacitors is demonstrated via simple and low‐cost spray painting of MoS₂ nanosheets on Si/SiO₂ chip and subsequent laser patterning. The obtained micro‐supercapacitors are well defined by ten interdigitated electrodes (five electrodes per polarity) with 4.5 mm length, 820 μm wide for each electrode, 200 μm spacing between two electrodes and the thickness of electrode is ～0.45 μm. The optimum MoS₂‐based micro‐supercapacitor exhibits excellent electrochemical performance for energy storage with aqueous electrolytes, with a high area capacitance of 8 mF cm^?2 (volumetric capacitance of 178 F cm^?3) and excellent cyclic performance, superior to reported graphene‐based micro‐supercapacitors. This strategy could provide a good opportunity to develop various micro‐/nanosized energy storage devices to satisfy the requirements of portable, flexible, and transparent micro‐electronic devices.     

Low‐Temperature Heteroepitaxy of 2D PbI2/Graphene for Large‐Area Flexible Photodetectors

Heterostructures based on graphene and other 2D atomic crystals exhibit fascinating properties and intriguing potential in flexible optoelectronics, where graphene films function as transparent electrodes and other building blocks are used as photoactive materials. However, large‐scale production of such heterostructures with superior performance is still in early stages. Herein, for the first time, the preparation of a submeter‐sized, vertically stacked heterojunction of lead iodide (PbI₂)/graphene on a flexible polyethylene terephthalate (PET) film by vapor deposition of PbI₂ on graphene/PET substrate at a temperature lower than 200 °C is demonstrated. This film is subsequently used to fabricate bendable graphene/PbI₂/graphene sandwiched photodetectors, which exhibit high responsivity (45 A W^?1 cm^?2), fast response (35 µs rise, 20 µs decay), and high‐resolution imaging capability (1 µm). This study may pave a facile pathway for scalable production of high‐performance flexible devices.     

Improving All‐Inorganic Perovskite Photodetectors by Preferred Orientation and Plasmonic Effect

All‐inorganic perovskites have high carrier mobility, long carrier diffusion length, excellent visible light absorption, and well overlapping with localized surface plasmon resonance (LSPR) of noble metal nanocrystals (NCs). The high‐performance photodetectors can be constructed by means of the intrinsic outstanding photoelectric properties, especially plasma coupling. Here, for the first time, inorganic perovskite photodetectors are demonstrated with synergetic effect of preferred‐orientation film and plasmonic with both high performance and solution process virtues, evidenced by 238% plasmonic enhancement factor and 10⁶ on/off ratio. The CsPbBr₃ and Au NC inks are assembled into high‐quality films by centrifugal‐casting and spin‐coating, respectively, which lead to the low cost and solution‐processed photodetectors. The remarkable near‐field enhancement effect induced by the coupling between Au LSPR and CsPbBr₃ photogenerated carriers is revealed by finite‐difference time‐domain simulations. The photodetector exhibits a light on/off ratio of more than 10⁶ under 532 nm laser illumination of 4.65 mW cm^?2. The photocurrent increases from 0.67 to 2.77 μA with centrifugal‐casting. Moreover, the photocurrent rises from 245.6 to 831.1 μA with Au NCs plasma enhancement, leading to an enhancement factor of 238%, which is the most optimal report among the LSPR‐enhanced photodetectors, to the best of our knowledge. The results of this study suggest that all‐inorganic perovskites are promising semiconductors for high‐performance solution‐processed photodetectors, which can be further enhanced by Au plasmonic effect, and hence have huge potentials in optical communication, safety monitoring, and biological sensing.     

A Metal–Organic‐Framework‐Based Electrolyte with Nanowetted Interfaces for High‐Energy‐Density Solid‐State Lithium Battery

Solid‐state batteries (SSBs) are promising for safer energy storage, but their active loading and energy density have been limited by large interfacial impedance caused by the poor Li⁺ transport kinetics between the solid‐state electrolyte and the electrode materials. To address the interfacial issue and achieve higher energy density, herein, a novel solid‐like electrolyte (SLE) based on ionic‐liquid‐impregnated metal–organic framework nanocrystals (Li‐IL@MOF) is reported, which demonstrates excellent electrochemical properties, including a high room‐temperature ionic conductivity of 3.0 × 10^‐4 S cm^‐1, an improved Li⁺ transference number of 0.36, and good compatibilities against both Li metal and active electrodes with low interfacial resistances. The Li‐IL@MOF SLE is further integrated into a rechargeable Li|LiFePO₄ SSB with an unprecedented active loading of 25 mg cm^‐2, and the battery exhibits remarkable performance over a wide temperature range from ?20 up to 150 °C. Besides the intrinsically high ionic conductivity of Li‐IL@MOF, the unique interfacial contact between the SLE and the active electrodes owing to an interfacial wettability effect of the nanoconfined Li‐IL guests, which creates an effective 3D Li⁺ conductive network throughout the whole battery, is considered to be the key factor for the excellent performance of the SSB.