Cross-linked Carbon Nanotubes Research Articles

Optimizing transparent electrodes: Interplay of high purity SWCNTs network and a polymer

The discovery of transparent electrodes led to the development of optoelectronic devices such as touchscreens, infrared (IR) sensors, etc. Carbon nanotubes (CNTs) have been a potential replacement for ITO due to their exceptional properties, especially in the IR region. In this work, we present the development of a CNT-polymer composite thin film that exhibits outstanding transparency across visible and IR spectra prepared by layer-by-layer (LbL) technique. This approach ensures uniform integration and crosslinking of CNTs into lightweight matrices, and also represents a cost-effective method for producing transparent electrodes with remarkable properties. The produced films achieved a transparency above 80 % in the UV/VIS range and approximately 70 % in the mid-IR range. The sheet resistance of the fabricated thin films was measured at about 4 kΩ/sq, showing a tendency to decrease with the number of bilayers. In this work we have investigated electrical properties and transport mechanisms in more detail with computational analysis. Computational analysis was performed to better understand the electrical behavior of nanotube-polymer junctions in the interbundle structure. Based on all results, we propose that the transparent electrodes with 4 and 6 bilayers are the most optimal structures in terms of optical and electrical properties.

Highly permeable carbon nanotube membranes for efficient surface water treatment through separation and adsorption–electrochemical regeneration

Membrane-based processes feature many advantages for surface water treatment over other technologies; however, the trade-off between membrane selectivity and permeability usually results in the failure to obtain high-quality filtrate at a high permeance. In this study, we report a highly permeable sodium alginate/glutaraldehyde cross-linked carbon nanotube (CNT/SA-GA) membrane with high adsorption ability for surface water treatment. The CNT/SA-GA membranes have a well-formed hollow fiber morphology and good conductivity of 166–261 S/m. They could reject >98 % of large-sized molecules (e.g., Alcian Blue 8GX and Congo Red) at high permeances of 137–227 L/(m2·h·bar). Moreover, they could remove ~100 % of smaller molecules (e.g., Rhodamine B (RhB)) through dynamic adsorption with a capacity of ~57.3 mg/g. Benefiting from their good conductivity, the CNT/SA-GA membranes could easily decompose the pollutants after adsorption saturation through electrochemical oxidation and then regenerated themselves. Though the switch between adsorption and electrochemical oxidation (2.0 V), the CNT/SA-GA membranes could remove ~100 % RhB at a high permeance of 342 L/(m2·h·bar), which is one order of magnitude higher than those of nanofiltration membranes. When used for surface water treatment, the CNT/SA-GA membranes exhibited a much higher TOC removal rate than commercial poly(acrylonitrile) (PAN) membranes (56.2 % vs. 7.2 %). LC-MS/MS analysis showed that many small molecules such as caffeine could be effectively removed by the CNT/SA-GA membranes. In addition, they exhibited a higher fouling resistance than PAN membranes, evidenced by their lower permeance decline ratio (10.1 % vs. 43.7 %). This study will promote the development and applications of the CNT-based membranes for water purification.

The configuration design of cross-linked CNT networks to realize heterostructure in Cu matrix composite towards prominent mechanical-electrical property synergy

Developing reticular reinforcement and heterogeneous microstructure remains persistent challenges in one-dimensional carbon nanotube (CNT)-Cu system. We herein fabricated dual-heterostructured Cu composite by diazotizing CNT into cross-linked (CL) networks and achieving bimodal grain distribution. The CL-CNT networks uniformly dispersed in Cu matrix, forming strong C–N/O–Cu covalent bonds at the interfaces and effectively retarding grain growth to create ultra-fine grain (UFG) regions around them. The CL-CNT networks/UFG regions, along with the surrounding coarse grain (CG) regions, resulted in a remarkable synergy between mechanical and electrical properties within the composite. Systematic analysis indicates that CL-CNT network acts as a whole to bear loading, remarkably enhances the load-transfer strengthening and promotes the dislocation accumulation around the interface. Meanwhile, hetero-deformation between “hard” CL-CNT networks/UFG regions and “soft” CG regions lead to extra-strengthening and hardening associated with strain partitioning, generation of geometrically necessary dislocation (GND) and strain delocalization. In-situ tensile test further reveals that CL-CNT/Cu with dual-heterostructure introduces the extra-toughening via crack bridging and deflection mechanisms. Besides, CL-CNT network with the robust interface is considered to reduce the interfacial inelastic scattering and provide additional paths for electron transport, accounting for the high electrical conductivity. This work highlights the importance of configuration design of reinforcement in tailoring heterostructured metal matrix composites (MMCs) with outstanding comprehensive performance.

Zirconium ion ligand Cross-Linked carbon nanotubes and leather collagen fibers for Flexible, Stable, and highly efficient underwater sensors

Flexible sensing materials have recently found widespread applications in integrating various underwater sensors. In this study, we adopted oil-tanned sheepskin as a “structural template” and harnessed its distinctive three-dimensional collagen fiber network. By leveraging the coordination complexation of zirconium ions (Zr4+), we brided collagen fibers with carbon nanotubes (CNTs) to enhance the bonding fastness of the two. We finally constructed a double cross-linked network to produce a new flexible conductive leather called CNTs@Zr@OTL. This material is the basis for preparing leather bio-based piezoresistive sensors （LBPS） and further developing leather biosensing systems (LBS). Experimental outcomes revealed that when CNTs were employed at a concentration of 8.5 %, CNTs@Zr@OTL exhibited an electrical resistivity of approximately 7.4 Ω·cm and a shrinkage temperature of around 74.5 °C. Furthermore, this material demonstrated remarkable characteristics, including 24-hour biodegradability, a broad sensing range (20 %-120 %), and high sensitivity (with response and recovery times of 300 ms and 100 ms, respectively). Based on multiple cross-linked networks, we propose for the first time the underwater sensing mechanism of “Submarine Tunnel” to achieve strong stability in the water environment. Finally, we simulated the LBPS's response to minor external stimuli, including rainwater exposure, multiangle reactions, and water depth sensitivity. By interfacing with wireless modules and mobile phones, the LBS enabled the execution of emergency SOS signals, highlighting its potential applications in underwater motion monitoring and urgent rescue operations.

Three-dimensional graphene cross-linked carbon nanotube doping as cathode for aqueous zinc ion batteries

Aqueous zinc ion batteries (ZIBs) are becoming increasingly popular in the field of energy storage due to their high safety and environmental friendliness. This study comparatively investigated the electrochemical performance of β-MnO2 as a cathode for ZIBs after doping with different ratios of three-dimensional graphene (3D-GPE)/carbon nanotube (CNT) cross-linked composite materials with ball milling. The results show that 3D-GPE/CNT cross-linked composite has an effect on β-MnO2 microstructure and particle morphology. The cathode made of β-MnO2/(3D-GPE/CNT) with a mass ratio of 9:1 has a very high reversible capacity of 1078.93 mAh/g at a current density of 10 mA g−1, which is about 2.24 and 1.87 times the other two ratio materials (18:1 and 12:1), respectively. After 100 cycles, the median voltage difference of the β-MnO2/(3D-GPE/CNT) mass ratio 9:1 specimen battery increased. The higher the median voltage, the higher the energy of the battery. The improvement of cathode performance is directly related to the micro-state, such as the three-dimensional frameworks and carbon nanotube structures of 3D-GPE/CNT, and the macro-state, such as particle refinement, homogenization, and layered structure.

Enhanced light-to-thermal conversion performance of self-assembly carbon nanotube/graphene-interconnected phase change materials for thermal-electric device

Solar energy conversion and storage technologies have attracted more attention to alleviate the energy crisis and ecological concern. Further improvement on the thermal conductivity and photothermal storage capacity of phase change materials (PCMs) remain a huge challenge. In this work, a new composite PCMs employing carbon-based (CRGO) aerogel as the supporting material and paraffin wax (PW) as the PCM was prepared. We achieve a three-dimensional (3D) porous interconnected structure by cross-linking carbon nanotubes (CNT) with reduced graphene oxide (rGO). This 3D structure could provide more heat transfer channels and effective contact interfaces, resulting in its enhanced thermal conductivity. The aspect ratio of CNT and the ratio of CNT and rGO is regulated to optimize the 3D thermal conductive skeleton for CRGO aerogel. As a result, the multi-layer CRGO aerogel composite PCMs exhibited high solid-liquid phase change enthalpy (146.7 J/g) and excellent phase change stability. Optimal incorporation of 30 % CNT increased the thermal conductivity to 1.27 W/(m·K), which is 452 % higher than that of the pure PW. Meanwhile, a photothermal conversion efficiency of up to 90.3 % was achieved for the composite PCMs. In addition, the output voltage of the solar-thermal-electric device based on composite PCMs (150 mV) is about 3.75 times that of the blank plate (40 mV) under solar radiation. Therefore, CRGO aerogel composite PCMs show great promise for efficient solar-thermal-electric energy conversion utilization.

Synergistic Effect of N-NiMoO4 /Ni Heterogeneous Interface with Oxygen Vacancies in N-NiMoO4 /Ni/CNTs for Superior Overall Water Splitting.

The exploring of economical, high-efficiency, and stable bifunctional catalysts for hydrogen evolution and oxygen evolution reactions (HER/OER) is highly imperative for the development of electrolytic water. Herein, a 3D cross-linked carbon nanotube supported oxygen vacancy (Vo )-rich N-NiMoO4 /Ni heterostructure bifunctional water splitting catalyst (N-NiMoO4 /Ni/CNTs) is synthesized by hydrothermal-H2 calcination method. Physical characterization confirms that Vo -rich N-NiMoO4 /Ni nanoparticles with an average size of ≈19nm are secondary aggregated on CNTs that form a hierarchical porous structure. The formation of Ni and NiMoO4 heterojunctions modify the electronic structure of N-NiMoO4 /Ni/CNTs. Benefiting from these properties, N-NiMoO4 /Ni/CNTs drives an impressive HER overpotential of only 46mV and OER overpotential of 330mV at 10mAcm-2 , which also shows exceptional cycling stability, respectively. Furthermore, the as-assembled N-NiMoO4 /Ni/CNTs||N-NiMoO4 /Ni/CNTs electrolyzer reaches a cell voltage of 1.64V at 10mAcm-2 in alkaline solution. Operando Raman analysis reveals that surface reconstruction is essential for the improved catalytic activity. Density functional theory (DFT) calculations further demonstrate that the enhanced HER/OER performance should be attributed to the synergistic effect of Vo and heteostructure that improve the conductivity of N-NiMoO4 /Ni/CNTs and facilitatethe desorption of reaction intermediates.

Electronic structure of carbon nanotube network

Covalently cross-linked carbon nanotube network has been synthesized using spark plasma sintering followed by nitric acid treatment. EPR investigation of its electronic structure in comparison with pristine carbon nanotubes has revealed that the covalent cross-linking leads to a decrease in the number of paramagnetic centers, while the oxidation results in an increase in their number. The oxidation affects the cross-linked and pristine materials in a different manner

Surface decoration of bis-aminosilane cross-linked multiwall carbon nanotube ultrafiltration membrane for fast and efficient heavy metal removal

Heavy metals (HMs) are highly toxic water pollutants abundant in industrial wastewater. Herein, a bis[3-(trimethoxysilyl)propyl]amine (BTMSPA) cross-linked multiwalled carbon nanotube (MWCNT) nanomaterial (CQACNT) was synthesized by silanization of MWCNT-OH followed by grafting of positively charged quaternary ammonium groups (glycidyl trimethyl ammonium chloride (GTMAC)) by an epoxide ring-opening reaction. The composite membranes were prepared by the incorporation of CQACNT into the poly(ether sulfone) (PES) polymer matrix. The CQACNT-6 composite membrane exhibited a 3.5-fold increase in pure water permeability (PWP; 312.8 L m−2 h−1 bar−1) as compared to the pristine PES (CQACNT-0) membrane (89.6 L m−2 h−1 bar−1). Moreover, the CQACNT-6 composite membrane showed high HM removal rates (Pb: 89.53%; Ni: 90.42%; Cu: 91.43%; Zn: 91.86%) as compared to the CQACNT-0 membrane (Pb: 39.73%; Ni: 40.32%; Cu: 42.52%; and Zn: 43.91%). After 9 treatment cycles, the CQACNT-6 membrane retained up to 87%, and 94% of its initial PWP and initial Cu2+ rejection, respectively, compared to only 58%, and 54%, respectively for pristine CQACNT-0. The positively charged quaternary ammonium groups enhanced the surface features of PES and MWCNTS, resulting in competitive HM removal rates due to the electrostatic repulsion between the HM and the porous membranes, as well as high PWP.

Carbon nano-structures and functionalized associates: Adsorptive detoxification of organic and inorganic water pollutants

• An overview of carbon-assisted materials for removal of different organic and inorganic pollutants. • Review of the key factors that affect adsorption performance. • Specific mechanism of interactions for different carbonaceous adsorbents. • Analysis of parameters and kinetics of adsorption. • The current hurdles and future insights to give overview on carbon-assisted materials for remediation of environmental pollutants. Deterioration of water quality is a desperate threat worldwide. Industrial development regularly added a vast amount of organic and inorganic contaminants to water. Therefore, eradicating these contaminants is highly essential for the well-being of biotic components. Adsorption-assisted technologies are among the most benign and principally used due to their higher efficiencies at lower costs and independence of complex technological supports. Carbon nanomaterials, such as activated carbons, carbon nanotubes, graphene-based materials, and carbon dots have been broadly adopted as adsorbents because of their outstanding surface characteristics. Researchers worked a lot on activation procedures and chemicals to achieve an ultrahigh surface area (above 3000 m 2 /g) to increase the adsorption efficiency. Further, cross-linked carbon nanotubes exhibited much-selected adsorption to organics. Carbon dots, a new type of carbon-based nanomaterials emerged as excellent adsorbents when introduced into the polymers matrix and provided promising platforms for the removal of metal ions. Also, graphene oxide and other oxidized forms of carbon being rich in functional groups are reported to exhibit excellent adsorption capacities as high as 2564 mg/g at 25 °C for basic and cationic compounds. Here, we reviewed the various types of pollutants found in aquatic biota with some basics on fundamentals and mechanistic features of adsorption, adsorption efficiency regulating factors. The article emphasized the performances of carbon nanomaterials and associated nanocomposites for the adsorption of various pollutants. The review also addresses the essential issues for the technical development and commercial application of carbon-assisted materials as nano adsorbents for water decontamination.

Vanadium hexacyanoferrate nanoparticles connected by cross-linked carbon nanotubes conductive networks for aqueous zinc-ion batteries

Prussian blue analogues (PBAs) have attracted increasing attention in the field of aqueous zinc-ion batteries (AZIBs) with the advantages of an open framework with adjustable valence and easy synthesis. However, due to the disadvantages of unstable structure and insufficient active sites, PBAs as cathode materials for AZIBs still have problems such as low specific capacity or poor cycle performance. In this work, a simple in-situ co-precipitation method is used to grow vanadium hexacyanoferrate (VHCF) nanoparticles on carbon nanotubes (CNTs), which aims to improve the conductivity of electrode materials by introducing a conductive skeleton of CNTs. This hybrid structure of VHCF nanoparticles and CNTs promotes electron transport between VHCF nanoparticles, thereby effectively improving the utilization of the material. Benefiting from the inherent sufficient channels for ions insertion/extraction of VHCF and the excellent conductivity of CNTs, the VHCF/CNTs hybrid as AZIBs cathode material shows excellent zinc storage performance with a high reversible capacity of 97.8 mAh g−1 at 50 mA g−1 and a discharge specific capacity of 52.7 mAh g−1 after 1000 cycles at 3200 mA g−1. This work provides a new idea for the design of high-performance PBAs-based cathodes for AZIBs.

Molecular dynamics simulation of cross-linked carbon nanotube for water treatment

Different carbon nanotube-based adsorbent materials have been prepared by chemical functionalization in recent years. Water treatment is the potential application because of their large special surface area, good mechanical properties and recyclability. In this work, molecular dynamics (MD) simulation is performed to investigate the adsorption of oil droplet from water by cross-linked carbon nanotubes (CL-CNTs). We have demonstrated that the factors of determining adsorption and recyclability capacity can be governed by controlling the length of cross-linker and the degree of cross-linking. The CL-CNTs exhibit good recyclability for oil molecules from wastewater. For different organic pollutants, the recyclability can be achieved through several procedures.

Carbon-coated MoS2 nanosheets@CNTs-Ti3C2 MXene quaternary composite with the superior rate performance for sodium-ion batteries

The exploration of advanced MoS2-based electrode materials overcoming their inherent low conductivity and large volume changes is of importance for next-generation energy storage. In this work, we report a simple and high-efficient one-pot hydrothermal approach to prepare a unique and stable 1D/2D heterostructure. In the architecture, ultrathin carbon layer-coated MoS2 nanosheets with large expanded interlayer of 1.02 nm are vertically grown onto the Ti3C2 MXene and cross-linked carbon nanotubes (CNTs), giving rise to a highly conductive 3D network. The interlayer expanded MoS2 nanosheets can greatly facilitate the Na ions/electrons transmission. Meanwhile, the N-doped 1D/2D CNTs-Ti3C2 matrix can be used as a strong mechanical support to well relieve the large volume expansion upon cycles. As a combination result of several advantages, the developed quaternary C-MoS2/CNTs-Ti3C2 composite anode shows an excellent sodium storage performance (562 mA h g−1 at 100 mA g−1 after 200 cycles) and rate capability (475 mA h g−1 at 2000 mA g−1). The density functional theory calculations further prove that the full combination of layer-expanded MoS2 nanosheets and N-doped Ti3C2 matrix can significantly enhance the adsorption energy of Na ions, further resulting in the enhancement of sodium storage capabilities.

Chirality-Dependent Mechanical Properties of Bundles and Thin Films Composed of Covalently Cross-Linked Carbon Nanotubes.

The effect of nanotube chirality on the mechanical properties of materials composed of single-walled carbon nanotubes (CNTs) is poorly understood since the interfacial load transfer in such materials is strongly dependent on the intertube interaction and structure of the nanotube network. Here, a combined atomistic-mesoscopic study is performed to reveal the effect of CNT diameter on the deformation mechanisms and mechanical properties of CNT bundles and low-density CNT films with covalent cross-links (CLs). First, the pullout of the central nanotube from bundles composed of seven (5,5), (10,10), (20,20), (17,0), and (26,0) CNTs is studied in molecular dynamics simulations based on the ReaxFF force field. The simulations show that the shear modulus and strength increase with decreasing CNT diameter. The results of atomistic simulations are used to parametrize a mesoscopic model of CLs and to perform mesoscopic simulations of in-plane tension and compression of thin films composed of thousands of cross-linked CNTs. The mechanical properties of CNT films are found to be strongly dependent on CNT diameter. The film modulus increases as the CNT diameter increases, while the tensile strength decreases. The in-plane compression is characterized by collective bending of whole films and order-of-magnitude smaller compressive strengths. The films composed of (5,5) CNTs exhibit the ability for large-strain compression without irreversible changes in the material structure. The stretching rigidity of individual nanotubes and volumetric CL density are identified as the key factors that dominate the effect of CNT chirality on the mechanical properties of CNT films. The film modulus is affected by both CL density and stretching rigidity of CNTs, while the tensile strength is dominated by CL density. The obtained results suggest that the on-demand optimization of the mechanical properties of CNT films can be performed by tuning the nanotube chirality distribution.

Less-Energy Consumed Hydrogen Evolution Coupled with Electrocatalytic Removal of Ethanolamine Pollutant in Saline Water over Ni@Ni3 S2 /CNT Nano-Heterostructured Electrocatalysts.

Energy crises, environmental pollution, and freshwater deficiency are critical issues on the planet. Electrolytic hydrogen generation from saline water, particularly from salt-contained hazardous wastewater, is significant to both environment and energy concerns but still challenging due to the high energy cost, severe corrosion, and the absence of competent electrocatalysts. Herein, a novel strategy is proposed for energy-efficient hydrogen production coupled with electro-oxidation removal of ethanolamine pollutant in saline water. To achieve this, an active and durable heterostructured electrocatalyst is developed by in situ growing Ni@Ni3 S2 core@shell nanoparticles in cross-linked 3D carbon nanotubes' (CNTs) network, achieving high dispersibility and metallic property, low packing density, and enriched exposed active sites to facilitate fast electron/mass diffusion. The unique Ni@Ni3 S2 /CNTs nano-heterostructures are competent for long-term stably electro-oxidizing environmental-unfriendly ethanolamine at a high current density of 100mA cm-2 in saline water, which not only suppresses oxygen and chloride evolution reactions but also decreases the energy consumption to boost hydrogen production. Associated with experimental results, density functional theory studies indicate that the collaborative adsorption of electrolyte ions and ethanolamine molecules can synergistically modulate the adsorption/desorption properties of catalytic active centers on Ni@Ni3 S2 /CNTs surface, leading to long-term stabilized electrocatalysis for efficient ethanolamine oxidation removal and less-energy hydrogen simultaneous production in saline water.

An adhesive and self-healable hydrogel with high stretchability and compressibility for human motion detection

Hydrogel strain sensors have attracted tremendous interest in artificial intelligence and human health monitoring for their large stretchability, good biocompatibility and self-healing capability. However, most epidermal strain sensors suffer from a poor device-skin interface, resulting in unreliability in the signal recording. Here, we prepared a self-adhesive, stretchable and compressible hydrogel consisting of dynamic cross-linked multi-walled carbon nanotubes , polyvinyl alcohol and polyacrylamide. The hydrogel formed a stable device-skin interface without any fixation assistance and thus allowed stable human motion signal recording from walking to facial expression. The hydrogel sensors exhibited a large sensing range of 500 % with a high gauge factor of 4.02 at 300–500 % tensile strain and a compressibility up to 70 %. In addition, the hydrogel is self-healable, and the conductivity of the hydrogel can be restored within 730 ms. At last, the hydrogel sensors were applied in human motion detection from vital throat vibration to walking, which paves the way for their practical applications in health monitoring and human-machine interactions.

Gas-Phase Oxidation of Spark Plasma Sintered Products of Covalently Crosslinked Carbon Nanotubes

Gas-Phase Oxidation of Spark Plasma Sintered Products of Covalently Crosslinked Carbon Nanotubes

Engineering Hierarchical Co@N-Doped Carbon Nanotubes/α-Ni(OH)2 Heterostructures on Carbon Cloth Enabling High-Performance Aqueous Nickel-Zinc Batteries.

Searching for high-performance Ni-based cathodes plays an important role in developing better aqueous nickel-zinc (Ni-Zn) batteries. For this purpose, herein, we demonstrate the design and synthesis of ultrathin α-Ni(OH)2 nanosheets branched onto metal-organic frameworks (MOFs)-derived 3D cross-linked N-doped carbon nanotubes encapsulated with tiny Co nanoparticles (denoted as Co@NCNTs/α-Ni(OH)2), which are directly supported on a flexible carbon cloth (CC). An aqueous Ni-Zn battery employing the hierarchical CC/Co@NCNTs/α-Ni(OH)2 as the binder-free cathode and a commercial Zn plate as the anode is fabricated, which displays an ultrahigh capacity (316 mAh g-1) and energy density (540.4 Wh kg-1) at 1 A g-1 as well as excellent rate capability (238 mAh g-1 at 10 A g-1) and superior cycling performance (about 84% capacity retention after 2000 cycles at 10 A g-1). The impressive electrochemical performance might benefit from the rich active sites, rapid electron transfer, cushy electrolyte access, rapid ion transport, and robust structural stability. In addition, the quasi-solid-state CC/Co@NCNTs/α-Ni(OH)2//Zn batteries are also successfully assembled with polymer electrolyte, indicating the great potential for portable and wearable electronics. This work might provide important guidance for constructing carbon-based hybrid materials directly supported on conductive substrates as high-performance electrodes for energy-related devices.

Fe-Nx doped carbon nanotube as a high efficient cathode catalyst for proton exchange membrane fuel cell

In this work, we report our recent efforts in developing carbon nanotube cross-linking MOF-derived Fe/N/C catalysts as oxygen reduction electrocatalysts for fuel cell. It is witnessed that the carbon nanotube cross-linking strategy can effectively improve the activity and stability of fuel cell, which can be assigned to its fast and convenient electron conduction channels offered by loosely cross-linked carbon nanotubes. The results of 57Fe Mössbauer spectroscopy show that there are three spin states of Fe-N4 structure in the material, of which low-spin state D1-FeIIN4 and high-spin state D3-N-FeN4 are both considered to be the main active sites of oxygen reduction reaction. For fuel cell, high performance of 0.732 A cm−2 at 0.7 V is reached. The novel cross-linking catalyst sheds light on the development of non-precious metal catalysts for fuel cells.

High-strength carbon nanotube/epoxy resin composite film from a controllable cross-linking reaction

Carbon nanotubes (CNTs) have been considered as potential reinforcements for various composites due to their excellent mechanical properties. However, it is still a challenge to prepare high-performance CNT/resin composites, resulting from the weak interfacial bonding between individual CNTs or that between CNTs and resin. Herein, a facile and effective method for preparing high-strength CNT/epoxy resin (EP) composite films is put forward, consisting of a controllable cross-linking treatment to the well-aligned CNT films and subsequent chemical filling with EP. Benefiting from the synergistic effects of optimized cross-linked CNTs and further enhancement by EP, the tensile strength of the obtained CNT/EP composite film reaches 2.5 GPa, which is about 5 times that of the raw CNT film. Our study might provide an effective strategy toward the preparation of high-performance CNT composite materials.