Thermal Management Properties Research Articles

Self-healing, adaptive and shape memory polymer-based thermal interface phase change materials via boron ester cross-linking

Addressing the thermal resistance between rough interfaces without applying pressure to the interfacial sandwich has been a challenge. Herein, a thermal interface phase change material (TIPCM) is designed to realize a 3D support skeleton with a dynamic crosslinking network by introducing a boron ester crosslinking backbone into paraffin wax (PW) and ethylene-octene copolymer (EOC), thus enabling the TIPCM to ensure mechanical integrity without leakage even above the melting temperature of EOC. The chemical cross-linking between the organic solid–liquid phase change material (PCM) and the polymer realizes thermally triggered self-healing and adaptive shape memory properties. The phase transition of PW leads to a decrease in the modulus of TIPCM and activates the ester exchange of the dynamic covalent bonding of boron esters, which allows TIPCM to self-heal and self-adapt to a variety of object surfaces. These enabled the TIPCM to fill the interface gaps through small stress deformations, forming an interlocking structure that reduces contact thermal resistance and promotes heat transfer. The obtained TIPCM achieves excellent chip thermal management performance, cooling the analog CPU temperature by 67 °C at 5 V. In conclusion, this study provides a potential strategy for redesigning TIPCMs with high latent heat and special physical properties for thermal management.

A regenerated cellulose fiber with high mechanical properties for temperature-adaptive thermal management.

The escalating global population has led to a surge in waste textiles, posing a significant challenge in landfill management worldwide. In this work, ionic liquid 1-butyl-3-methylimidazole acetate ([Bmim]OAc) and DMF (N, n-dimethylformamide) were used as solvents to dissolve waste denim fabric, then vanadium dioxide (VO2) nanoparticles were introduced into the spinning solution, and cellulose fibers were regenerated by dry-wet spinning process, to promote the recycling of waste cotton fabric. Finally, regenerated cellulose fibers with high added value were prepared by dry-wet spinning. Through this innovative strategy, on the one hand, because VO2 can form a large number of hydrogen bonds between the regenerated cellulose molecules, and realize the cross-networking structure of the molecular chains inside the fiber, the mechanical properties of the regenerated cellulose fibers are enhanced. On the other hand, due to the thermal phase transformation characteristics of VO2, it also endows the regenerated cellulose fiber unique intelligent temperature control function. Compared with the pristine regenerated fiber, the tensile stress of the regenerated fiber after adding VO2 nanoparticles (F-VO2) increased by 25.6%, reaching 158.68MPa. In addition, the F-VO2 fibric provides excellent intelligent temperature control, reducing temperatures by up to 6.7°C.

Cellulose–derived carbon scaffolds with bidirectional gradient Fe3O4 distribution: Integration of green EMI shielding and thermal management

Cellulose papers (CPs) possess a pore structure, rendering them ideal precursors for carbon scaffolds because of their renewability. However, achieving a tradeoff between high electromagnetic shielding effectiveness and low reflection coefficient poses a tremendous challenge for CP-based carbon scaffolds. To meet the challenge, leveraging the synergistic effect of gravity and evaporation dynamics, laminar CP-based carbon scaffolds with a bidirectional gradient distribution of Fe3O4 nanoparticles were fabricated via immersion, drying, and carbonization processes. The resulting carbon scaffold, owing to the bidirectional gradient structure of magnetic nanoparticles and unique laminar arrangement, exhibited excellent in-plane electrical conductivity (96.3 S/m), superior electromagnetic shielding efficiency (1805.9 dB/cm2 g), low reflection coefficients (0.23), and a high green index (gs, 3.38), suggesting its green shielding capabilities. Furthermore, the laminar structure conferred upon the resultant carbon scaffold a surprisingly anisotropic thermal conductivity, with an in-plane thermal conductivity of 1.73 W/m K compared to a through-plane value of only 0.07 W/m K, confirming the integration of thermal insulation and thermal management functionalities. These green electromagnetic interference shielding materials, coupled with thermal insulation and thermal management properties, hold promising prospects for applications in sensitive devices.

Self-healing, adaptive and shape memory polymer-based thermal interface phase change materials via boron ester cross-linking

Addressing the thermal resistance between rough interfaces without applying pressure to the interfacial sandwich has been a challenge. Herein, a thermal interface phase change material (TIPCM) is designed to realize a 3D support skeleton with a dynamic crosslinking network by introducing a boron ester crosslinking backbone into paraffin wax (PW) and ethylene-octene copolymer (EOC), thus enabling the TIPCM to ensure mechanical integrity without leakage even above the melting temperature of EOC. The chemical cross-linking between the organic solid–liquid phase change material (PCM) and the polymer realizes thermally triggered self-healing and adaptive shape memory properties. The phase transition of PW leads to a decrease in the modulus of TIPCM and activates the ester exchange of the dynamic covalent bonding of boron esters, which allows TIPCM to self-heal and self-adapt to a variety of object surfaces. These enabled the TIPCM to fill the interface gaps through small stress deformations, forming an interlocking structure that reduces contact thermal resistance and promotes heat transfer. The obtained TIPCM achieves excellent chip thermal management performance, cooling the analog CPU temperature by 67 °C at 5 V. In conclusion, this study provides a potential strategy for redesigning TIPCMs with high latent heat and special physical properties for thermal management.

Low-temperature strain-free encapsulation for perovskite solar cells and modules passing multifaceted accelerated ageing tests

Perovskite solar cells promise to be part of the future portfolio of photovoltaic technologies, but their instability is slow down their commercialization. Major stability assessments have been recently achieved but reliable accelerated ageing tests on beyond small-area cells are still poor. Here, we report an industrial encapsulation process based on the lamination of highly viscoelastic semi-solid/highly viscous liquid adhesive atop the perovskite solar cells and modules. Our encapsulant reduces the thermomechanical stresses at the encapsulant/rear electrode interface. The addition of thermally conductive two-dimensional hexagonal boron nitride into the polymeric matrix improves the barrier and thermal management properties of the encapsulant. Without any edge sealant, encapsulated devices withstood multifaceted accelerated ageing tests, retaining >80% of their initial efficiency. Our encapsulation is applicable to the most established cell configurations (direct/inverted, mesoscopic/planar), even with temperature-sensitive materials, and extended to semi-transparent cells for building-integrated photovoltaics and Internet of Things systems.

Bioinspired composite fiber aerogel pressure sensor for machine-learning-assisted human activity and gesture recognition

Machine-learning-assisted human activity and gesture recognition are valuable for human-computer interaction, and data acquisition often necessitates high-performance sensors. Here, inspired by spider web and bat wing airflow sensing system, polyimide fiber (PIF)/carbon black (CB) composite fiber aerogel (CFA) pressure sensor with biomimetic hair-Merkel cell sensitive unit was developed, exhibiting ultralow detection limit (2 Pa), high pressure sensitivity (S=23.1 kPa-1), wide linear detection capacity up to 67.61 kPa, and fast response/recovery time (140/100 ms). Thanks to the excellent mechanical property and environmental tolerance of CFA, it also possesses excellent low fatigue over >4000 cycles and good durability even at extreme high-temperature (200 °C) and underwater conditions. The superior signal data of the sensor, combined with the Convolutional Neural Network machine learning algorithm, achieves ultra-high prediction accuracies of 96.73% and 98.26% for human activity and gesture recognition, respectively. Additionally, CFA also has amazing thermal management properties, making it to be an ideal candidate for wearable electronics with excellent wearing comfort and safety.

Multi-heterointerface integration in nitrogen-doped Ti3C2Tx@Fe3O4 nanocomposites for superior microwave absorption

Engineering a lightweight and thin microwave absorber through the design of multiple heterogeneous interfaces represents a significant challenge. Here, we synthesized a nitrogen (N)-doped Ti3C2Tx@Fe3O4 (N–Ti3C2Tx@Fe3O4) nanocomposite with a sandwich-like structure through a solvothermal approach using hydrazine hydrate as the N donor. The numerous Ti3C2Tx electron transfer pathways of Ti3C2Tx enable the realization of a hierarchical conduction network within N–Ti3C2Tx@Fe3O4. The introduction of defects through N doping and the integration of Fe3O4 with Ti3C2Tx are pivotal for enhancing the dipole polarization. The heterogeneous interfaces in N–Ti3C2Tx@Fe3O4, coupled with Fe3O4 components, substantially boost the electromagnetic wave (EMW) absorption performance of the composite. An optimal N integration and the loading of Fe3O4 in Ti3C2Tx result in an improved impedance matching of N–Ti3C2Tx@Fe3O4. The synergistic effect of the improved impedance matching and the strong EMW attenuation capability endow N–Ti3C2Tx@Fe3O4 with enhanced microwave absorption (MA) properties. Specifically, at a thickness of 1.04 mm, the composite exhibits the effective absorption bandwidth (3.92 GHz; 14.08–18.00 GHz), surpassing that of Ti3C2Tx. At a thickness of 0.98 mm, it exhibits a maximum reflection loss of −40.28 dB at 17.25 GHz, which substantially exceeds that of Ti3C2Tx. Furthermore, it shows a maximum Radar Cross Section reduction of 21.32 dB cm2. A cotton fabric was coated with N–Ti3C2Tx@Fe3O4, and it was found to exhibit enhanced heat conduction and dissipation, at rates 3.83 and 4.64 times greater than those of uncoated cotton, respectively. These results highlight the considerable potential of N–Ti3C2Tx@Fe3O4 nanocomposites for use in far-field applications. It is envisaged that the exceptional MA and thermal management properties of N–Ti3C2Tx@Fe3O4 nanocomposites will provide a novel avenue for crafting lightweight and thin EMW absorbing materials.

Construction of 3D BN network with high-density thermal conductive paths

Efficient heat dissipation is essential to further improve the integration of high-power electronic packaging devices. Three-dimensional BN networks with high-density thermal conductive paths were designed as the heat transfer skeleton of thermal interface materials. 3D networks with high-density thermal conductive paths inlaid between oriented BN paths were constructed using precursor self-assembly and freeze-drying to improve the thermal conductivity of polymeric materials. The results show that high-density thermally conductive paths have stronger polymer-enhanced thermal conductivity than directional thermal paths and compared with pure TPU, the thermal conductivity of TPU/BN-2 under low BN filling content (10%wt) is increased by 250 % and 286.5 % in the through surface and flat surface respectively. This work provides new ideas for the preparation of polymer composites for thermal interface materials in electronic packaging and integrated circuits with excellent thermal management properties.

Multiple birds with one stone: A new type of PPy/Fe3O4/rGO multifunctional composite fabric for wave absorption, UV resistance, anti-static and thermal insulation

To solve the problem of electromagnetic radiation pollution, it is especially important to develop electromagnetic wave-absorbing materials with excellent performance. The preparation of composite multifunctional textile materials with excellent wave-absorbing properties is one of the research hotspots for practical personal protection applications. In this work, PPy/Fe3O4/rGO polyester/cotton composite fabrics were prepared by impregnation, chemical reduction, chemical co-precipitation and in situ polymerization. When the thickness is 0.97 mm, the minimum reflection loss (RLmin) of PPy/Fe3O4/rGO polyester/cotton composite fabric is −12.12 dB, and the effective absorption bandwidth (EAB) is 4.7 GHz, which is excellent in wave absorption. Meanwhile, the PPy/Fe3O4/rGO polyester/cotton composite fabrics have excellent UV resistance (UV transmittance ratio of UVA and UVB bands as low as 0.02 %, UPF value of 100+), antistatic properties (static voltage half-life of 0.2 s), and excellent thermal management properties (thermal conductivity as low as 0.05796 W/(m·K)), and so on. The PPy/Fe3O4/rGO polyester/cotton composite fabrics prepared in this study are suitable for a variety of application scenarios, such as individual electromagnetic protection, individual protection in extremely cold environments, and individual heating physiotherapy, which is of great reference significance for the research of wearable individual protective textile materials.

Fabrication of High Thermal Conductivity Aluminum Nitride Ceramics via Digital Light Processing 3D Printing.

The sintering of high-performance ceramics with complex shapes at low temperatures has a significant impact on the future application of ceramics. A joint process of digital light processing (DLP) 3D printing technology and a nitrogen-gas pressure-assisted sintering method were proposed to fabricate AlN ceramics in the present work. Printing parameters, including exposure energy and time, were optimized for the shaping of green bodies. The effects of sintering temperature, as well as nitrogen pressure, on the microstructure, density, and thermal conductivity of AlN ceramics were systematically discussed. A high thermal conductivity of 168 W·m-1·K-1 was achieved by sintering and holding at a significantly reduced temperature of 1720 °C with the assistance of a 0.6 MPa nitrogen-gas pressure. Further, a large-sized AlN ceramic plate and a heat sink with an internal mini-channel structure were designed and successfully fabricated by using the optimized printing and sintering parameters proposed in this study. The heat transfer performance of the ceramic heat sink was evaluated by infrared thermal imaging, showing excellent cooling abilities, which provides new opportunities for the development of ceramic heat dissipation modules with complex geometries and superior thermal management properties.

A novel nanohybrid, Fe3O4/NHS@M(OH)(OCH3)@rGO (M= Co, Ni), with petal-shaped anisotropic interfaces imparts efficient EMW absorption, flame retardancy, and thermal management properties to epoxy resin

As epoxy resin (EP) is widely used in the microelectronic field, it is essential to improve its electromagnetic wave (EMW) absorption and flame retardancy simultaneously. In this work, we synthesized a novel nanohybrid, RMN (Fe3O4/NHS@M(OH)(OCH3)@rGO (M = Co, Ni)), with petal-shaped anisotropic interfaces, by using graphene oxide as the core and the 2D nanosheets M(OH)(OCH3) (M = Co, Ni) as the petal, with nickel hydroxystannate and ferrite as further modifications. The RMN combines carbon-based materials, ferrites and conductors, and represents the petal-like structure with rich nondirectional interfaces. The results show that EP composite containing 25 wt% RMN represented excellent EMW absorption, with a minimum reflection loss of −55.79 dB (with 7.4 mm thickness at 3.1 GHz). Moreover, the EP composite with 15 wt% RMN (EP/RMN700-3) had the lowest peak heat release rate of 470.9 kW m−2, which was 69.7 % lower than pure EP, showing a significantly improving in flame retardant. The thermal conductivity efficiency of EP/RMN700-3 increased to 128.4 % compared with the pure EP, which effectively reduces fire risk caused by heat accumulation. This study provides a valuable solution to overcome the challenges of EMW absorption and flame retardant for EP in the microelectronic materials field.

Deep eutectic supramolecular polymer functionalized MXene for enhancing mechanical properties, photothermal conversion, and bacterial inactivation of cellulose textiles

Two-dimensional (2D) transition metal carbides (Ti3C2Tx MXene) have gained significant attention for their potential in constructing diverse functional materials, However, MXene is easily oxidized and weakly bound to the cellulose matrix, which pose challenges in developing MXene-decorated non-woven fabric with strong bonding and stable thermal management properties. Herein, we successfully prepared deep eutectic supramolecular polymer (DESP) functionalized MXene to address these issues. MXene can be wrapped with DESP to be insulated from water and protected from being oxidized. Subsequently, we achieved an efficient in-situ deposition of DESP-functionalized MXene onto fibers through a combination of dip coating and photopolymerization technique. The resulting nonwoven fabric (CNs-DESP@M) exhibited excellent photothermal conversion properties along with rapid thermal response and functional stability. Interestingly, the interface bonding between MXene and the fiber surface was significantly enhanced due to the abundant pyrogallol groups in DESP, resulting in the composite textile exhibiting commendable mechanical properties (2.68 MPa). Moreover, the as-prepared textile demonstrates outstanding bactericidal efficacy against both Escherichia coli (E. coli) and Staphylococcus aureus (S. aureus). The multifunctional textile, created through a facile and efficient approach, demonstrates remarkable potential for applications in smart textiles, catering to the diverse needs of individuals in the future.

Vitrimeric phase change material facilitating 3D-structured boron nitride network for reliable thermal conductive interface materials

Phase change materials (PCMs) shows great promise as thermal interface materials (TIMs) due to their compliance and thermal management properties from solid-liquid phase transition characteristics. However, the significantly reduced thermal conductivity resulting from that randomly dispersed thermal conductive fillers susceptible to localized volume change by solid-liquid phase transition deteriorates the reliable heat transfer of TIM but is often overlooked. In this work, 3D-structured network of boron nitride (BN) fillers is created in vitrimeric PCM (vPCM) consisting of dynamic covalent crosslinked polyolefin elastomer (POE)/paraffin wax (PW) blends. The resulted composites with interconnected BN network show a through-plane thermal conductivity (κ⊥) of 3.08 W m−1 K−1 at 29.8 vol% BN. Significantly, the composites can keep the BN network continuous when heated, and remain κ⊥ of about 1.4 W m−1 K−1 after the solid-liquid phase transition of PW, which ensures reliable heat transfer when achieving thermal management by melting endotherm of PW. Moreover, the composites conform to the surface topography of sandwiching surfaces through solid plasticity under low stress when the crosslinked network rearranges via the exchange of dynamic covalent bonds activated by the melting of POE, reducing the thermal contact resistance. When the composites are used as TIM through thermally triggered reconfigurable package procedures at 80 °C and 50 kPa, the heat dissipation is better than a commercial thermal pad with κ⊥ of 3.86 W m−1 K−1. Vitrimeric PCM facilitates reliable 3D-structured BN network and thermally triggered conformability, paving a promising way for high-performance TIM with excellent heat dissipation.

Polyimide aerogels with a dual electrically conductive network for electromagnetic interference shielding, piezoresistive sensing, and thermal management

The constant iteration of wearable devices necessitates lightweight electromagnetic shielding materials with multiple functions. In this study, an elastic reduced graphene oxide/polyimide (rGO/PI) aerogel skeleton was prepared through freeze-drying and thermal annealing. Then the highly conductive two-dimensional (2D) transition metal carbide (MXene) was coated onto the rGO/PI skeleton using vacuum impregnation to fabricate MXene@rGO/PI composite aerogels. Due to the dual electrically conductive network formed by rGO and MXene, the MXene@rGO/PI composite aerogels exhibit exceptional electromagnetic interference shielding effectiveness (EMI SE) of 58.7 dB in the X-band at a density of 0.063 g cm−3. Additionally, these composite aerogels demonstrate sensitive piezoresistive sensing capabilities (the electrical resistance variation caused by compressive stress) for detecting human body motion and also possess excellent thermal management properties including efficient Joule heating (up to 108 °C at 10 V) and superior thermal insulation performance. This work presents a feasible strategy for developing polymer-based composites for multi-functional applications such as wearable electronics.

Self-Adaptive Rapid Thermal Conductive Fabrics Based on Hygroscopic Shrinkage Response for Personal Cooling and Drying.

Advanced fabrics with thermal wet management capability as low energy consumption media contribute to personal cooling and drying. Nevertheless, it remains a great challenge to obtain intelligent fabrics with adjustable thermal conductivity (TC) capable of bridging the supply and demand between human body temperature and self-adaptive thermal conduction. Herein, we report hygroscopic-shrinkage nanofiber-based fabrics with excellent moisture sensitivity and significant volume shrinkage, which benefits the construction of high-density thermal conductive pathways by absorbing sweat, with a maximum sweat absorption rate reaching up to 1781%. The TC of the shrunken fabric is significantly increased from the initial 0.102 to 0.731 W·m-1 K-1 with a volume shrinkage rate of 89% due to the synergistic effect of van der Waals force, capillary force, viscous resistance, and gravity. Besides, an enhanced TC of the resulting fabrics facilitates rapid heat transfer to the environments. By capturing the surface temperature variations of the fabric after shrinkage and commercially available cotton/Coolmax, we obtained the fabric that releases the same amount of heat in a shorter period of time (3.3 s). With its exceptional personal thermal and wet management properties, this study paves the way for designing new-generation intelligent fabrics capable of creating more comfortable microclimates.

Bionic-leaf vein inspired breathable anti-impact wearable electronics with health monitoring, electromagnetic interference shielding and thermal management

Breathable and stretchable conductive materials are ideal for healthcare wearable electronic devices. However, the tradeoff between the sensitivity and detection range of electronic sensors and the challenge posed by simple-functional electronics limits their development. Here, inspired by the bionic-leaf vein conductive path, silver nanowires (AgNWs)-Ti3C2Tx (MXene) hybrid structure assembled on the nonwoven fabrics (NWF) is well sandwiched between porous polyborosiloxane elastomer (PBSE) to construct the multifunctional breathable wearable electronics with both high anti-impact performance and good sensing behavior. Benefiting from the high conductive AgNWs-MXene hybrid structure, the NWF/AgNWs-MXene/PBSE nanocomposite exhibits high sensitivity (GF = 1158.1), wide monitoring range (57 %), controllable thermal management properties, and excellent electromagnetic interference shielding effect (SET = 41.46 dB). Moreover, owing to the wonderful shear stiffening effect of PBSE, the NWF/AgNWs-MXene/PBSE possesses a high energy absorption performance. Combining with deep learning, this breathable electronic device can be further applied to wireless sensing gloves and multifunctional medical belts, which will drive the development of electronic skin, human-machine interaction, and personalized healthcare monitoring applications.

Asymmetric Janus Fibers with Bistable Thermochromic and Efficient Solar–Thermal Properties for Personal Thermal Management

Asymmetric Janus Fibers with Bistable Thermochromic and Efficient Solar–Thermal Properties for Personal Thermal Management

Composite phase change materials with thermal-flexible and efficient photothermal conversion properties for solar thermal management

Composite phase change material (CPCM) with the advantages of high enthalpy and constant temperature phase change, has been widely used in many fields, such as photovoltaic thermal system, building envelope structure and so on. However, conventional CPCM is often rigid, poor light absorption and low thermal conductivity, which limits the application of solar energy utilization. In this paper, a novel Paraffin wax/Thermoplastic elastomer/Carbon nanotube(PA/SEBS/CNT) with shape stability, thermos-flexibility and high photothermal conversion efficiency was prepared, PA as the phase change material, SEBS as the flexible material and CNT as the light-absorbing material. The results show that the addition of CNT increases the absorbance of PA/SEBS from 0.3 to 1.0, and the photothermal conversion efficiency of PA/SEBS/CNT-10 % is as high as 96.17 %. In addition, the CPCM also has a high enthalpy value of 180 J/g, and a high thermal conductivity of >0.3403 W/(m·K), and also exhibits shape-driven memory. At the same time, outdoor photothermal experiments show that PA/SEBS/CNT has excellent photothermal conversion performance under real sunlight, and the highest temperature can reach 99.51 °C. The new CPCM developed has a broad application prospect in solar thermal systems.

Stretchable and lightweight 2D MXene-based elastomeric composite foam for suppressing electromagnetic interference

The utilization of lightweight materials that provide electromagnetic interference (EMI) shielding and impact attenuation is crucial for safeguarding fragile components in portable electronic devices. Although conductive foams have shown promise in providing lightweight electromagnetic interference (EMI) shielding, their potential for impact attenuation has yet to be thoroughly investigated. In this study, we fabricated a composite foam consisting of MXene and carboxylated nitrile rubber (MXene/XNBR) to achieve multifunctional properties such as electromagnetic interference (EMI) shielding and thermal management. The fabrication method involved the utilization of MXene nanoflakes and XNBR elastomer through a dual mixing approach, which encompassed both melt and solution mixing techniques. Utilizing a chemical blowing agent in integrating cellular structure inside a composite material has resulted in several advantageous properties, including reduced weight, enhanced processability, and improved thermal management capabilities. The MXene/XNBR foam composite exhibits a higher EMI shielding efficiency (SE) of − 30.9 dB. With a remarkably low density of 0.7 g.cm−3, this material exhibits a specific shielding effectiveness of 441.4 dB.cm2.g−1 with desirable stretchability and mechanical strength, positioning it as one of the most promising options for lightweight applications. Our multifunctional elastomeric foam composites collectively offer a significant pathway for developing high-performance foam material that exhibits exceptional shielding efficiency, thermal management, stretchability, and superior mechanical properties.

Devisable pore structures and tunable thermal management properties of aerogels composed of carbon nanotubes and cellulose nanofibers with various aspect ratios

The anisotropic cellulose nanofiber (CNF)/carbon nanotube (CNT) aerogels hold a great promise in directional applications due to their distinct xylem-like aligned penetrating pore structures. The aspect ratio of CNF plays a crucial role in the pore structures of aerogels, directly dominating the final macroscopic properties of materials. Herein, three types of CNF with different aspect ratios were extracted through the 2,2,6,6-tetrmethylpiperidine-1-oxyl radical (TEMPO) oxidation process by changing the doses of oxidant. The corresponding anisotropic CNF/CNT aerogels were prepared by the unidirectional freeze-drying method and then their pore morphologies and properties were investigated in detail. The resulting aerogel with the shortest aspect ratio of CNF exhibited the densest porous structure, thereby obtaining the highest compressive strength of 110 kPa and elastic modulus of 383 kPa, while that containing the longest CNF possessed the highest thermal conductivity coefficient of 0.17 W m−1 K−1 and the worst thermal insulation. This research explored the relationship between the properties of the CNF/CNT aerogels and devisable pore structures caused by various aspect ratios of CNF, thus providing a new insight into the development of CNF/CNT aerogels with tunable performances.