Flexible Electronic Materials Research Articles

A Semi‐Interpenetrating Poly(Ionic Liquid) Network‐Driven Low Hysteresis and Transparent Hydrogel as a Self‐Powered Multifunctional Sensor

AbstractConductive hydrogels are gaining significant attention as promising candidates for the fabrication materials for flexible electronics. Nevertheless, improving the tensile properties, hysteresis, durability, adhesion, and electrochemical properties of these hydrogels remains challenging. This work reports the development of a novel semi‐interpenetrating network poly(ionic liquid) hydrogel named PATV, via the in situ polymerization of acrylamide, N‐[Tris(hydroxymethyl)methyl] acrylamide, and 1‐vinyl‐3‐butylimidazolium tetrafluoroborate. The density functional theory calculations reveal that the poly(ionic liquid) in the hydrogel network acts as physical cross–linking points to construct hydrogen‐bond networks. Furthermore, the hydrogen‐bond networks dissipate energy efficiently and quickly, and thus stress concentration and hysteresis are avoided. The prepared hydrogel has a low hysteresis (9%), high tensile properties (900%), fast response (180 ms), high sensitivity (gauge factor = 10.4, pressure sensitivity = 0.14 kPa−1), and wide sensing range (tensile range: 1–600%, compression range: 0.1–20 kPa). A multifunctional sensor designed based on the designed hydrogel enables real‐time, rapid, and stable response‐ability for the detection of human movement, facial expression recognition, pronunciation, pulse, handwriting, and Morse code encryption. Furthermore, the assembled triboelectric nanogenerator displays an excellent energy harvesting capability, thus highlighting its potential application in self‐powered flexible wearable electronic devices.

Epoxy Resins with Controllable "Thermally Conductive-Self-Healing" Synergies: a New Material to Meet the Needs of Flexible Electronic Devices.

With the popularization of 5G technology and artificial intelligence, thermally conductive epoxies with self-healing ability will be widely used in flexible electronic materials. Although many compounds containing both performances have been synthesized, there is little systematic theory to explain this coordination mechanism. In this paper, alkyl chains of different lengths were introduced to epoxies for discussing the thermally conductive, the self-healing performance, and the synergistic effect. A series of electronic-grade biphenyl epoxies (4,4'-bis(oxiran-2-ylmethoxy)-1,1'-biphenyl (1), 4,4'-bis(2-(oxiran-2-yl)ethoxy)-1,1'-biphenyl (2), 4,4'-bis(3-(oxiran-2-yl)propoxy)-1,1'-biphenyl (3), and 4,4'-bis(4-(oxiran-2-yl)butoxy)-1,1'-biphenyl (4) were synthesized and characterized. Furthermore, they were cured with decanedioic acid to produce polymers. Results showed that alkyl chains can both affect the two properties, and the epoxies suitable for specific application scenarios can be prepared by adjusting the length of alkyl chains. In terms of thermal conductivity, compound 1 was a most promising material. However, compound 4 was expected to be utilized in flexible electronic devices because of its acceptable thermal conductivity, self-healing ability, transparency, and flexibility.

Xylan‑Assisted construction of anisotropic aerogel for pressure sensor

Currently, aerogels are promising for wearable pressure sensors due to their superior flexibility and high sensitivity. However, uniform dispersion of conductive solid filler is a critical step in the preparation process. Herein, xylan with good amphiphilicity was obtained by hydroxypropylsulfonation under mild reaction conditions, which is accepted as a dispersant for multi-walled carbon nanotubes (MWCNTs) in water. The hydroxypropylsulfonated xylan (HSX) exhibited a satisfactory dispersion efficiency reached to 97.8 %. After standing for 20 days, there are still 76 % of MWCNTs stabilized in the dispersion. Then, the ultralight, flexible and superstable anisotropic aerogels were prepared by freeze-casting technology. The obtained aerogel reveals excellent mechanical performance, with a great compressibility (undergoing a strain of 70 %) and elasticity (91.8 % height retention after 100 cycles at a strain of 20 %). As a proof of concept, the HSX/MWCNTs aerogel is utilized to construct a pressure sensor, which exhibit high sensitivity (S = 2.17 kPa−1) and impressive responsiveness to human motions. This work demonstrates a promising flexible electronic material for wearable electronics, electronic skin, and human motion monitoring.

Constructing a 3D Ion Transport Channel-Based CNF Composite Film with an Intercalated Structure for Superior Performance Flexible Supercapacitors.

The weak stiffness, huge thickness, and low specific capacitance of commonly utilized flexible supercapacitors hinder their great electrochemical performance. Learning from a biomimetic interface strategy, we design flexible film electrodes based on functional intercalated structures with excellent electrochemical properties and mechanical flexibility. A composite film with high strength and flexibility is created using graphene (reduced graphene oxide (rGO)) as the plane layer, layered double metal hydroxide (LDH) as the support layer, and cellulose nanofiber (CNF) as the connection agent and flexible agent. The interlayer height can be adjusted by the ion concentration. The highly interconnected network enables excellent electron and ion transport channels, facilitating rapid ion diffusion and redox reactions. Moreover, the high flexibility and mechanical properties of the film achieve multiple folding and bending. The CNF-rGO-NiCoLDH film electrode exhibits high capacitance performance (3620.5 mF cm-2 at 2 mA cm-2), excellent mechanical properties, and high flexibility. Notably, flexible all-solid assembled CNF-rGO-NiCoLDH//rGO has an extremely high area energy density of 53.5 mWh cm-2 at a power density of 1071.2 mW cm-2, along with cycling stability of 89.8% retention after 10 000 charge-discharge cycles. This work provides a perspective for designing high-performance energy storage materials for flexible electronics and wearable devices.

Unconventional mechanical and thermal behaviours of MOF CALF-20.

CALF-20 was recently identified as a benchmark sorbent for CO2 capture at the industrial scale, however comprehensive atomistic insight into its mechanical/thermal properties under working conditions is still lacking. In this study, we developed a general-purpose machine-learned potential (MLP) for the CALF-20 MOF framework that predicts the thermodynamic and mechanical properties of the structure at finite temperatures within first-principles accuracy. Interestingly, CALF-20 was demonstrated to exhibit both negative area compression and negative thermal expansion. Most strikingly, upon application of the tensile strain along the [001] direction, CALF-20 was shown to display a distinct two-step elastic deformation behaviour, unlike typical MOFs that undergo plastic deformation after elasticity. Furthermore, this MOF was shown to exhibit a fracture strain of up to 27% along the [001] direction at room temperature comparable to that of MOF glasses. These abnormal thermal and mechanical properties make CALF-20 as attractive material for flexible and stretchable electronics and sensors.

Shutters-Inspired metal ions coordination hydrogel Strain/Pressure sensor for joint behavior evaluation and flatfeet correction

The metal ions coordination hydrogels (MI-HG) that polymer gels serve as flexible substrates and metal ions as conductive media have emerged as flexible electronic sensor materials. Nevertheless, fabricating MI-HG by a traditional soaking method is difficult to guarantee the good permeation of metal ions, manifesting as the “core–shell” structure of MI-HG, which undoubtedly reduces their mechanical property, conductivity, and sensitivity. Inspired by the shutter opening and closing regulation mechanism, a strategy that completely opening the backbone layers of polymer gels facilitates metal ions permeation thus improving the whole performance of MI-HG, especially the mechanical property is proposed. Herein, poly(vinyl alcohol)(poly(acrylic acid)-polyacrylamide) (PVA(PAA-PAM)) is used as the typical polymer hydrogel (HG), trivalent aluminum ion (Al3+) as the metal salt, and N,N'-methylenebisacrylamide (MBAA) as the important regulation ‘rod’, fabricating a series of aluminum coordination hydrogels (Al-HGx%). The results indicate that the mechanical performances of Al-HG2% are significantly improved. For example, the toughness of Al-HG2% reaches 996.12 KJ/m3, approximately three times that of the Al-HG0% sample (354.45 KJ/m3). The combination of structural characterization as well as finite element analysis, the mechanism for the enhanced mechanical performances based on shutter’s completely open effect is elucidated, the product of which (Al-HG2%) has potential application in flexible strain/pressure sensor for joint behavior evaluation and flatfeet correction.

Flexible electronic materials and devices toward portable immunoassays

AbstractBiomarker identification is a tried‐and‐true method that can provide precise biological information for disease diagnosis. Prompt diagnosis, disease progression monitoring, therapy efficacy evaluation, and prognosis assessment of cancers all benefit from sensitive, rapid, and precise measurement of significant biomarkers employing chemical and immunological approaches. The study of biomolecules and immunoassay evaluations can profit greatly from recent advancements in flexible electronic materials and technologies, which provide amazing flexibility, affordability, mobility, and integration. However, an overview of the implementation of portable immunoassays in conjunction with flexible electronic devices is rare to come by. This review focuses on recent breakthroughs in flexible electronic materials and devices for portable biomarker testing, which provides an extensive summary of flexible electrical components and sensing‐capable devices, emphasizing their adaptability in the construction of biosensing platforms. These platforms employ various signal transduction systems to record biological affinity recognition events, including pressure, temperature, electrical parameters, colorimetric signals, and other physical features. The challenges for portable, integrated, intelligent, and multifunctional immunoassays based on flexible sensing devices are also discussed. The portable immunoassays with flexible electronics would unlock the potential to transform clinical diagnostics into non‐clinical personalized treatments and achieve home‐based point‐of‐care testing for daily monitoring.

Electronic Properties of CrB/Co2CO2 Superlattices by Multiple Descriptor-Based Machine Learning Combined with First-Principles.

In recent times, newly unveiled 2D materials exhibiting exceptional characteristics, such as MBenes and MXenes,have gained widespread application across diverse domains, encompassing electronic devices, catalysis, energy storage, sensors, and various others. Nonetheless, numerous technical bottlenecks persist in the development of high-performance, structurally flexible, and adjustable electronic device materials. Research investigations have demonstrated that 2D van der Waals superlattices (vdW SLs) structures comprising materials exhibit exceptional electrical, mechanical, and optical properties. In this work, the advantages of both materials are combined and compose the vdW SLs structure of MBenes and MXenes, thus obtaining materials with excellent electronic properties. Furthermore, it integrates machine learning (ML) with first-principles methods to forecast the electrical properties of MBene/MXene superlattice materials. Initially, various configurations of MBene/MXene superlattice materials are explored, revealing that distinct stacking methods exert significant influence on the electronic structure of MBene/MXene materials. Specifically, the BABA-type stacking of CrB (layer A) and Co2CO2 MXene (layer B) is most stable configureation. Subsequently, multipledescriptors of the structure are constructed to predict the density of states of vdW SLs through the employment of MLtechniques. The best model achieves a mean absolute error (MAE) as low as 0.147 eV.

Smart materials for flexible electronics and devices: hydrogel.

In recent years, flexible conductive materials have attracted considerable attention for their potential use in flexible energy storage devices, touch panels, sensors, memristors, and other applications. The outstanding flexibility, electricity, and tunable mechanical properties of hydrogels make them ideal conductive materials for flexible electronic devices. Various synthetic strategies have been developed to produce conductive and environmentally friendly hydrogels for high-performance flexible electronics. In this review, we discuss the state-of-the-art applications of hydrogels in flexible electronics, such as energy storage, touch panels, memristor devices, and sensors like temperature, gas, humidity, chemical, strain, and textile sensors, and the latest synthesis methods of hydrogels. Describe the process of fabricating sensors as well. Finally, we discussed the challenges and future research avenues for flexible and portable electronic devices based on hydrogels.

Elastic and conductive gellan gum/polyvinyl alcohol physical hydrogels with low swelling potential for sustainable flexible electronics

Conductive hydrogels are considered to be promising materials for flexible electronics, but those nondegradable are bound to produce substantial undesirable electronic wastes once widely applied, inconsistent with the long-term sustainable development goals. To develop biodegradable conductive hydrogels for sustainable flexible electronics, a green chemical reaction-free strategy was developed to manufacture a novel type of composite hydrogels, exploiting biodegradable gellan gum and polyvinyl alcohol as the matrices and natural-derived tannic acid as the crosslinking agent. The technique involves successive cool-induced sol−gel transition, freeze-thawing and Na2SO4 solution treatment. A universal electronic testing machine, scanning electronic microscope, X-ray diffractometer, thermogravimetric analyzer, and electrochemical work station were employed to study the mechanics, structure and morphology, swelling and conductivity of the hydrogels. The results indicate strong, elastic and tough hydrogels were achieved owing to the multi-crosslinked multiple-network structure. The maximum compressive stress (90% strain), tensile strength, breakage elongation and fracture energy reach 10.7 MPa, 1.2 MPa, 890% and 480 kJ/m3 respectively. The stress recovery rate still remains 86% after 10 consecutive loading-unloading under 200% strain. The highest conductivity reaches 3.27 S/m, which along with the excellent mechanics confers them good strain-sensing behavior. Moreover, the final hydrogels show low swelling in both water (the equilibrium swelling ratio (ESR) < 300%) and physiological saline (ESR < 90%). The excellent mechanical performance, high conductivity and good strain sensing, low swelling and inherent biodegradability as well as the ecofriendly manufacturing process imply potential prospect in sustainable flexible electronics.

Influence of SrTiO3/Fe2O3 nano-fillers assisted PVDF-HFP polymer nanocomposite films on dielectric, impedance, and conductivity studies for energy storage applications

abstract In recent years, electronic devices with trendy flexibility and compatibility have become the competitive alternative to conventional electronics. In the present work, flexible polymer nanocomposite films composed of poly(vinylidene fluoride-co-hexafluoropropylene), iron oxide, and strontium titanate (PVDF-HFP/SrTiO3/Fe2O3) were synthesized by the solution-casting method. The formation and structural features of this composite material have been analyzed by X-Ray diffraction (XRD), Fourier transform infrared spectroscopy (FTIR), Thermogravimetric (TGA), and SEM. SEM results confirm the homogeneous dispersion of SrTiO3 and Fe2O3 within the host polymer. The uniform dispersion of the embedded metal species enhances the dielectric values up to 462 on optimization with infused rigidity. The impedance studies of PVDF-HFP/SrTiO3/Fe2O3 were performed in the temperature region of 50–150 °C at various frequencies ranging from 50 Hz to 10 MHz and the AC conductivity studies suggested that synthesized polymer nanocomposite shows higher conductivity with the maximum conductivity value was 8.20 × 10−3S/m. Polymer nanocomposite films with large dielectric constant and minimum dielectric loss are highly recommendable for flexible energy storage applications. Also, rapid development of novel material for flexible electronics is in great demand, which suggests it is an alternate source for future energy storage application.

Liquid Metal Powders Wrapped with Robust Shell by Bimetallic Ions Chelation Strategy for Energy Harvesting and Flexible Electronics

AbstractExcellent electrical and fluidic properties render liquid metal (LM) a promising material for flexible electronics, soft robotics, and stretchable circuits. Although producing LM micro/nano droplets by nanometerization addresses the tricky issue of the processing result from high surface tension, it still remains challenging to obtain stable LM droplets because of their dynamic surfaces. In this study, LM powders wrapped with robust shells are fabricated by bimetallic ions chelation strategy. During sonicating LM (e.g., EGaIn) in an alginate solution, a microgel shell is first formed by the coordination of Ga3+ and carboxyl groups. Subsequently, LM powders are achieved by introducing Ca2+ as secondary metal ions to chelate with redundant carboxyl groups. Besides high chemical stability in water and air, these nonstick LM powders also exhibit superior photothermal effects for energy harvesting, being capable of recovering electrical conductivity by mechanical sintering for flexible electronics. These conductive circuits based on LM powders not only work as electro‐thermal heaters, and electromagnetic interference shielding material but also can be designed as smart actuators. Thus, this bimetallic ions chelation strategy may start a pathway to produce stable, transportable LM powders with multifunctional properties, applicable in stretchable electronics, smart actuators, and electric skins.

Laser-Based Additive Nanomanufacturing: Rigid to Flexible Substrates

Current printed electronics manufacturing techniques, including inkjet and aerosol jet printing, use ink to produce electronics devices. The inks are formulated with pigments, additives, and solvents, which make the inks impure. Also, small changes in the composition of the inks will result in different chemical and physical properties, which might affect the printing process as well as the final performance of the device. In addition, the ink formulations are rather complex, with a limited source of functional materials for printing functional devices. Annealing during printing or post-processing for solvent removal is another challenge of these techniques, which limit printing on low temperature and biodegradable substrates. Herein, we present a novel additive nanomanufacturing (ANM) technique compatible with a wide range of substrates for dry printing and patterning of a variety of materials, including on different rigid and flexible substrates. Bending tests show good mechanical stability and electrical conductivity, confirming the potential of ANM technique for printing different materials for flexible hybrid electronics and sensors.

2D Materials in Flexible Electronics: Recent Advances and Future Prospectives.

Flexible electronics have recently gained considerable attention due to their potential to provide new and innovative solutions to a wide range of challenges in various electronic fields. These electronics require specific material properties and performance because they need to be integrated into a variety of surfaces or folded and rolled for newly formatted electronics. Two-dimensional (2D) materials have emerged as promising candidates for flexible electronics due to their unique mechanical, electrical, and optical properties, as well as their compatibility with other materials, enabling the creation of various flexible electronic devices. This article provides a comprehensive review of the progress made in developing flexible electronic devices using 2D materials. In addition, it highlights the key aspects of materials, scalable material production, and device fabrication processes for flexible applications, along with important examples of demonstrations that achieved breakthroughs in various flexible and wearable electronic applications. Finally, we discuss the opportunities, current challenges, potential solutions, and future investigative directions about this field.

3D printing and freeze casting hierarchical mxene pressure sensor

Although MXene sheets are highly conductive, it is still challenging to prepare MXene complex functional materials for flexible electronics by simple and effective methods. In 3D printing, especially direct ink writing (DIW), different materials are used to create complex 3D shapes by formulating inks with controlled rheological properties. Herein, a printable MXene ink is developed, exhibiting good rheological properties, to print different complex shapes, and potentially manufacture electronic devices such as sensors. Then, we fabricated a highly sensitive hierarchical structure MXene composite materials composed of two layers of bionic micro-spine microstructure and network structure, formed by 3D printing and freeze casting. The obtained MXene composite materials exhibit good pressuring sensing properties with a sensitivity of 17.5 kPa−1, a fast response time (<100 ms), and excellent cycle stability exceeding 10,000 cycles. The sensing mechanism suggesting that the hierarchical structure can effectively improve the sensitivity and response time. It also has good potential application in the monitoring of human health activities, including the detection of human joint activities, walking, pressure distribution, and other sports.

Immobilizing Polyiodides with Expanded Zn2+ Channels for High‐Rate Practical Zinc‐Iodine Battery

AbstractAqueous zinc‐iodine battery (AZIB) has the advantage of low cost and high specific capacity but suffer from the soluble polyiodides shuttling and sluggish redox kinetics. Herein, these two limitations are addressed by employing a cathode additive (zirconium hydrogen phosphate, denoted as EI‐ZrP) which provides dual functions: an agent for polyiodide confinement, and abundant channels for zinc ion transport. An enlarged crystalline interlayer (from typical 7.5 to 18.3 Å) of the EI‐ZrP significantly enhances the ionic conductivity and simultaneously immobilizes polyiodides, leading to an accelerated conversion process. AZIB with EI‐ZrP in the iodine cathode exhibits a high capacity retention over 10,000 cycles (with a 0.02‰ decay rate per cycle). Quasi‐solid‐state Zn‐I2 pouch cell has been constructed using hydrogel‐paper as separator and EI‐ZrP additive, which delivers a high areal capacity under repeated bending. As a proof‐of‐concept demonstration, the paper battery is integrated to power a wireless flexible pressure sensor system (WFPSS). This strategy may shed light on the rational design of conversion‐type cathode materials for both energy storage and flexible portable electronics.

A temperature and pressure dual-responsive, stretchable, healable, adhesive, and biocompatible carboxymethyl cellulose-based conductive hydrogels for flexible wearable strain sensor

The study aimed to develop a novel temperature and pressure dual-responsive conductive hydrogel with self-healing, self-adhesive, biocompatible, and stretchable properties, for the development of multifunctional anti-counterfeiting and wearable flexible electronic materials. A conductive hydrogel based on carboxymethyl cellulose (CMC) was synthesized by simple “one pot” free radical polymerization of CMC, acrylamide (AAm) and acrylic acid (AAc). The hydrogel displayed temperature responsiveness and possessed an upper critical solution temperature (UCST) value. In addition, hydrogels also had surprising pressure responsiveness. The synthesized hydrogels were characterized by FTIR, TGA, DSC, and XRD analysis. Importantly, the obtained hydrogels exhibited exceptional mechanical properties (stress: 730 kPa, strain: 880%), fatigue resistance, stretchability, self-healing capability, self-adhesive properties, and conductivity. In addition, valuable insights were obtained into the synthesis and application of flexible anti-counterfeiting and camouflage materials by the temperature and pressure dual-responsive hydrogels. Moreover, the prepared hydrogel, with an electrically sensitive perception of external strain (GF = 2.61, response time: 80 ms), can be utilized for monitoring human movement, emotional changes, physiological signals, language, and more, rendering it suitable for novel flexible anti-counterfeiting materials and versatile wearable iontronics. Overall, this study provided novel insights into the simple and efficient synthesis and sustainable manufacturing of environmentally friendly multifunctional anti-counterfeiting materials and flexible electronic skin sensors.

Composite polymeric film for stretchable, self-healing, recyclable EMI shielding and Joule heating

Although the electromagnetic interference (EMI) shielding materials have attracted much attention in recent years, it is still a big challenge to develop EMI materials with stretchable, self-healing and recyclable property, realizing reliable usage and avoiding electronic waste. In this paper, we have developed a multifunctional elastomeric adhesive called MFEA, which comprises polydimethylsiloxane, dimethylacetohydrazide/4,4-methylene bis(phenyl isocyanate), and catechol. MFEA exhibits outstanding mechanical performance(3.75 MPa), strong adhesion(1 MPa), self-healing capabilities(91 %), and recyclability. By leveraging its adhesive properties, we can combine MFEA with silver nanowires. The composite MFEA/AgNWs film not only exhibits outstanding performance, including stretchability, self-healing, adhesion, and recyclability, but can also be used to manufacture EMI shielding films with an shielding strength of up to 53.6 dB. Additionally, the composite film exhibits Joule heating behavior, rapidly heating to over 50 ℃ under a 1.5 V and maintaining stability for an extended duration. Moreover, MFEA can be used to adhere to other commercial EMI shielding films to achieve desired functionalities using conventional methods. This approach provides a universal, convenient, and rapid strategy for preparing flexible electronic materials with various functionalities.

High‐Resolution Intaglio Transfer Printing of Silver Nanowires for Wearable Electrophysiological Sensors

Silver nanowires (NWs) are promising materials for flexible electronics, such as electronic skins due to their excellent electrical, thermal, and mechanical properties. Achieving precise patterning of Ag NWs is essential for the successful integration and miniaturization of the electronic device system, but the high aspect ratio (AR) of NWs and the high porosity of NW networks pose challenges in forming high‐resolution patterns. Herein, the intaglio transfer printing technique to create high‐resolution patterning of ultralong Ag NWs (AR≈1000) is presented. During the pattern formation process, the external force becomes concentrated specifically at the edge of the intaglio trench, resulting in the breaking of the entangled Ag NW network in the corresponding region. This simple yet effective technique enables precise high‐resolution (minimum line width: 7 µm) and complicated Ag NW patterns on flexible substrates. The patterned Ag NWs are conformally attached to the various curvilinear surfaces and show high mechanical stability under continuous bending conditions. Wearable electrophysiological sensors are demonstrated to monitor electromyography and electrocardiogram signals in real‐time for continuous healthcare monitoring. This patterning strategy offers an effective approach for achieving high‐resolution patterns of highly anisotropic nanomaterials and highlights the potential of patterned Ag NWs in wearable electronics.

Two‐dimensional Ti3C2Tx (MXene)‐multiwalled carbon nanotubes reinforced ethyl methyl acrylate/ethylene octene copolymer binary blend hybrid nanocomposites with enhanced thermal and dielectric properties

AbstractPolymer composites with high dielectric constant and minimal dielectric losses have wide ranging prospects for advanced applications in the flexible electronics and electrical industry. In this study, we used the advantages of carbonaceous hybrid nanofillers to develop a flexible dielectric material. Herein, a set of hybrid nanocomposites were successfully fabricated by incorporating the Ti3C2Tx (MXene) and MWCNTs (multi‐walled carbon nanotubes) hybrid mixture as the conductive moiety into the poly(ethylene‐co‐methyl acrylate) (EMA)/ethylene‐octene co‐polymer (EOC) binary blend as the matrices using solution mixing technique followed by compression molding. As prepared, EMA/EOC/Ti3C2Tx/MWCNTs hybrid composites have been characterized by FTIR (Fourier transform infrared) spectroscopy, XRD (X‐ray diffraction), TGA (thermogravimetric analysis), FESEM (field emission scanning electron microscopy), and DSC (differential scanning calorimetry). We studied the effects of Ti3C2Tx and MWCNTs contents in the hybrid composites on the thermal, dielectric, and electrical properties. Among all the 15 wt% hybrid mixture containing 2 wt% MWCNTs loaded composite has the highest dielectric constant (ℇr = 122.21) and the lowest dissipation loss (tan δ = 0.030) at 100 Hz. The present studies recommend the EMA/EOC/Ti3C2Tx/MWCNTs hybrid composites can be used in smart and flexible electronic storage material.Highlights EMA‐EOC blend composites with hybrid Ti3C2Tx/MWCNTs were processed. 2.5 wt% MWCNTs loaded hybrid composite shows excellent thermal stability. Composite with 2 wt% MWCNTs has ℇ' = 122.21 and tanδ = 0.03 at 100 Hz. 2.5 wt% MWCNTs composite has electrical conductivity of 3.26 × 10−8 Ω−1 m−1. This composite can be used in smart and flexible electronic storage material.