Polymer Composite Films Research Articles

Electrically Insulating Flexible Films with Quasi-1D van der Waals Fillers as Efficient Electromagnetic Shields in the GHz and Sub-THz Frequency Bands.

Polymer composite films containing fillers comprising quasi-1D van der Waals materials, specifically transition metal trichalcogenides with 1Dstructural motifs that enable their exfoliation into bundles of atomic threads, are reported. These nanostructures are characterized by extremely large aspect ratios of up to ≈106 . The polymer composites with low loadings of quasi-1D TaSe3 fillers (<3vol%) reveal excellent electromagnetic interference shielding in the X-band GHz and extremely high frequency sub-THz frequency ranges, while remaining DC electrically insulating. The unique electromagnetic shielding characteristics of these films are attributed to effective coupling of the electromagnetic waves to the high-aspect-ratio electrically conductive TaSe3 atomic-thread bundles even when the filler concentration is below the electrical percolation threshold. These novel films are promising for high-frequency communication technologies, which require electromagnetic shielding films that are flexible, lightweight, corrosion resistant, inexpensive, and electrically insulating.

Tailoring the photoluminescent and electrical properties of tin-doped ZnS@PVP polymeric composite films for LEDs applications

Abstract In the present work, tailoring the photoluminescent and electrical properties of Zn1-xSnxS@PVP polymeric composite films has been achieved for LEDs applications. Un-doped and 1.0 wt % of Sn-doped ZnS in polyvinyl pyrrolidine (Zn1-xSnxS@PVP) polymeric composite films were prepared using solution casting technique. The effect of Sn molar ratio x (x: 0 to 0.3) on the morphological, structural, photoluminescent and electrical properties is explored using a scanning electron microscope, X-ray diffraction (XRD), photoluminescence (PL) and DC electrical conductivity studies. XRD measurements reveal the amorphous nature of both bare PVP and Zn1-xSnxS@PVP polymeric composite films. The PL spectra measurements of the prepared films exhibit broad emission peaks with maxima intensities ranged from 400 to 417 nm. The Gaussian fitting method is used to de-convolute the PL emission bands of bare PVP and Zn1-xSnxS@PVP polymeric composite films. Three emission peaks for ZnS@PVP polymeric film are noticed at 392, 430 and 476 nm. An extra emission peak located at the green light region (480–502 nm) is observed for Zn1-xSnxS@PVP composite films. The electrical conductivity of the prepared Zn1-xSnxS@PVP polymeric composite films is enhanced thirty times more than that of bare PVP one. The prepared Zn1-xSnxS@PVP polymeric composite films could play an important role in LEDs applications.

Enhanced dielectric and electrical properties of tri-phase percolative PVDF–BiFeO3–Carbon Black (CB) composite film

A tri-phase polymer composite film with a multiferroic phase (BiFeO3) and conductive carbon black (CB) deposited on the BiFeO3 (BF) and poly(vinylidene fluoride) (PVDF) matrix were prepared by using a solution casting technique. The dielectric and electrical performance of BF–PVDF composites with various weight percentages of CB content was studied. It has been observed that the incorporation of high loading of CB to the BF–PVDF composite system led to a significant improvement in the dielectric constant with suppressed dielectric loss (< 0.5). The high dielectric constant of 69 at 100 Hz, which is 11 times greater than that of neat PVDF film with a lower dielectric loss of 0.41, is obtained for PVDF–BF–CB composites as CB content (8 wt%) approached the percolation threshold. Furthermore, the improvement of dielectric and electrical performance of the PVDF–BF–CB composites may be due to the synergistic effect of the multiferroic phase BF and conductive phase CB as a result of homogeneous dispersion within the polymer matrix. These high dielectric constant and suppressed dielectric loss PVDF–BF–CB composites might be suitable for potential applications in the field of future thin-film capacitors.

Flexible and thin multifunctional waterborne polyurethane/Ag film for high-efficiency electromagnetic interference shielding, electro-thermal and strain sensing performances

With the rapid development of the flexible electronics industry, the range of multifunctional applications of materials has become extensive. But it is still a challenge to apply flexible materials to different fields while ensuring corresponding performance. Herein, a simple and available approach is addressed to fabricate conductive polymer composite films supported on Ag flakes and waterborne polyurethane (WPU) by spraying. The WPU/Ag films with uniform structure show outstanding flexibility and electromagnetic interference shielding effectiveness of 68.9 dB with thickness of only 50 μm, and could sustain a high standard even undergoing excessive mechanical deformations. Besides, the resulted films possess prominent electro-thermal effect, which can achieve a temperature of over 120 °C by applying a low voltage of 2 V, and the heat can be dissipated rapidly along with the connecting Ag network. Moreover, it shows a high gauge factor (229.2), good durability and reproductivity (over 1000 cycles), and rapid response time to strain (50 ms), which can be potentially used in the field of human movement monitoring and wearable electronic devices. These results indicate the multifunction of the WPU/Ag film, which could widen its practical applications after the corresponding treatment.

Incorporating MXene into Boron Nitride/Poly(Vinyl Alcohol) Composite Films to Enhance Thermal and Mechanical Properties.

Aggregated boron nitride (ABN) is advantageous for increasing the packing and thermal conductivity of the matrix in composite materials, but can deteriorate the mechanical properties by breaking during processing. In addition, there are few studies on the use of Ti3C2 MXene as thermally conductive fillers. Herein, the development of a novel composite film is described. It incorporates MXene and ABN into poly(vinyl alcohol) (PVA) to achieve a high thermal conductivity. Polysilazane (PSZ)-coated ABN formed a heat conduction path in the composite film, and MXene supported it to further improve the thermal conductivity. The prepared polymer composite film is shown to provide through-plane and in-plane thermal conductivities of 1.51 and 4.28 W/mK at total filler contents of 44 wt.%. The composite film is also shown to exhibit a tensile strength of 11.96 MPa, which is much greater than that without MXene. Thus, it demonstrates that incorporating MXene as a thermally conductive filler can enhance the thermal and mechanical properties of composite films.

A Crystalline Three-Dimensional Covalent Organic Framework with Flexible Building Blocks.

The construction of three-dimensional covalent organic frameworks (3D COFs) has proven to be very challenging, as their synthetic driving force mainly comes from the formation of covalent bonds. To facilitate the synthesis, rigid building blocks are always the first choice for designing 3D COFs. In principle, it should be very appealing to construct 3D COFs from flexible building blocks, but there are some obstacles blocking the development of such systems, especially for the designed synthesis and structure determination. Herein, we reported a novel highly crystalline 3D COF (FCOF-5) with flexible C-O single bonds in the building block backbone. By merging 17 continuous rotation electron diffraction data sets, we successfully determined the crystal structure of FCOF-5 to be a 6-fold interpenetrated pts topology. Interestingly, FCOF-5 is flexible and can undergo reversible expansion/contraction upon vapor adsorption/desorption, indicating a breathing motion. Moreover, a smart soft polymer composite film with FCOF-5 was fabricated, which can show a reversible vapor-triggered shape transformation. Therefore, 3D COFs constructed from flexible building blocks can exhibit interesting breathing behavior, and finally, a totally new type of soft porous crystals made of pure organic framework was announced.

Radiation-Induced Improving Mechanical and Thermal Properties of Carboxymethyl Cellulose/Clay Composite for Application in Removal of Copper(II) Ions from Wastewater

A study was carried out on the effect of gamma irradiation on the mechanical and thermal properties of carboxymethyl cellulose (CMC)/Ca-montmorillonite clay composite, prepared by blending using solvent method. In this study, carboxymethyl cellulose was used as a hosting matrix where clay was added to there at different contents: 0.25, 0.5, 1, 1.5 wt%, as a filler. The polymer composite films were cross-linked by irradiation with different integral doses. The results showed that the tensile strength (TS) increased continuously with radiation dose up to 10 kGy, beyond which declined. Meanwhile, TS exhibited increases with clay load ratio. However, the elongation at break (Eb) decreased continuously with dose and clay percentage within the developed composite films. Variation in structure and thermal properties were studied using X-ray diffractometion (XRD), scanning electron microscopy (SEM), Fourier-transform infrared spectroscopy (FTIR) and thermogravimetric analysis (TGA) techniques. The produced CMC/clay composites were implemented in removing copper (II) ions from a synthesized wastewater. The isotherm models and kinetic studies for the adsorption of Cu (II) onto CMC/clay were carried out. The results revealed that 0.1 g fabricated composite film irradiated at 10 kGy significantly removed copper (II) ions with adsorption capacity of 54.6 mg/g at optimum conditions: pH = 5, contact time = 300 min.

Significant Reduction of Interfacial Thermal Resistance and Phonon Scattering in Graphene/Polyimide Thermally Conductive Composite Films for Thermal Management.

The developing flexible electronic equipment are greatly affected by the rapid accumulation of heat, which is urgent to be solved by thermally conductive polymer composite films. However, the interfacial thermal resistance (ITR) and the phonon scattering at the interfaces are the main bottlenecks limiting the rapid and efficient improvement of thermal conductivity coefficients (λ) of the polymer composite films. Moreover, few researches were focused on characterizing ITR and phonon scattering in thermally conductive polymer composite films. In this paper, graphene oxide (GO) was aminated (NH2-GO) and reduced (NH2-rGO), then NH2-rGO/polyimide (NH2-rGO/PI) thermally conductive composite films were fabricated. Raman spectroscopy was utilized to innovatively characterize phonon scattering and ITR at the interfaces in NH2-rGO/PI thermally conductive composite films, revealing the interfacial thermal conduction mechanism, proving that the amination optimized the interfaces between NH2-rGO and PI, reduced phonon scattering and ITR, and ultimately improved the interfacial thermal conduction. The in-plane λ (λ||) and through-plane λ (λ⊥) of 15 wt% NH2-rGO/PI thermally conductive composite films at room temperature were, respectively, 7.13 W/mK and 0.74 W/mK, 8.2 times λ|| (0.87 W/mK) and 3.5 times λ⊥ (0.21 W/mK) of pure PI film, also significantly higher than λ|| (5.50 W/mK) and λ⊥ (0.62 W/mK) of 15 wt% rGO/PI thermally conductive composite films. Calculation based on the effective medium theory model proved that ITR was reduced via the amination of rGO. Infrared thermal imaging and finite element simulation showed that NH2-rGO/PI thermally conductive composite films obtained excellent heat dissipation and efficient thermal management capabilities on the light-emitting diodes bulbs, 5G high-power chips, and other electronic equipment, which are easy to generate heat severely.

Dispersion of Nano-materials in Polymer Composite Materials

Polymer composites materials are the subject of extensive studies because of their novel properties compared with their constituent materials. Dispersion stability of sub-micron sized particles in the medium is important from the point of colloidal views. In the present study, dispersion of nano-materials in the matrix polymer is one of the most important problems to enhance their mechanical properties. We tackled this problem to carry out surface modification of the nano-materials, such as carbon nano tubes (CNTs), using amphiphilic polymers, polyNvinylacetamide (PNVA), synthesized thorough radical polymerization. Hydrogen bond worked between PNVA onto the modified nano-materials and hydrophilic matrix, such as polyvinyl alcohol (PVA), to enhance surface adhesions and dispersions of the nano-materials in the matrix. As a result, the mechanical properties of their composites materials were strengthened. When CNTs were used in PVA, the transparency of the composite was also increased due to improvement of their dispersions. In addition, if the CNTs formed the networks in the composites, the highly conductive and transparent polymer composite films were fabricated.

Preparation of ZnO nanoparticles modified with silane coupling-agents to fabricate anti-UV Poly(vinyl chloride) films.

The uses of inorganic metal oxide as ultraviolet (UV) absorbers have potential to increase the production of UV protection and can also overcome the disadvantages of organic molecules. In this article, we report an effective technique to fabricating polyvinyl chloride (PVC) films with well UV shielding efficiency. Surface modification of zinc oxide (ZnO) nanoparticles (NPs) with different silane coupling-agents were achieved, and through solution casting technique dispersed within the PVC matrix. Infrared spectroscopy (FT-IR), scanning electron microscopy (SEM), thermogravimetric analysis (TGA) and UV spectrophotometer were applied to study the structures, dispersions, and optical properties. The results showed that the functionalized ZnO NPs could be well dispersed in PVC and endow the polymer composite films with significantly improved anti-UV capability. The facile processing and obtained properties of PVC composites have shown potential for low cost and environmentally sustainable applications in the UV protection field.

Free volume dependence of dielectric behaviour in sandwich-structured high dielectric performances of poly(vinylidene fluoride) composite films.

A dielectric film with a trilayer structure is fabricated to obtain both a high dielectric constant and superior electrical breakdown strength simultaneously. The outer layers of the trilayered composite film are composed of barium titanate (BTO) particles dispersed in poly(vinylidene fluoride) (PVDF) to ensure a relatively high dielectric constant, while the central layer of the composite film consists of exfoliated hexagonal boron nitride nanosheets (BNNS) dispersed in PVDF to provide high electrical breakdown strength. Compared with pristine PVDF, the dielectric constant and breakdown strength are simultaneously enhanced due to the sandwich structure, and the dielectric loss is maintained at a low level. Most important of all, positron annihilation lifetime spectroscopy (PALS) is applied to study the atomic-scale free volume holes of PVDF composite films and the effect of free volume holes on the dielectric constant and breakdown strength. Results show that the size of free volume holes of PVDF increased with the addition of BTO, but it decreased firstly and then increased with the BNNS loading. The correlation between dielectric properties and the size of free volume holes of the PVDF matrix was discussed in each layer. It is illustrated that the experimental dielectric constant of the PVDF/BTO single-layered film is consistent with the theoretical value at a lower BTO loading but smaller than the theoretical value at a higher BTO loading, which is probably ascribed to the increased size of free volume holes. The breakdown strength of the PVDF/BNNS film increased with the introduction of BNNS and the reduced size of free volume holes, which is ascribed to the reduced partial discharge phenomenon. The atomic-scale microstructure analysis based on free volume holes provides valuable ideas and new understanding for the study of the mechanism of the dielectric behaviour of polymer composites.

PVDF/CNF/IL composite film for shielding of microwave radiation

In this work materials have been used in the form of conducting polymer composite film for covering of different electrical and electronic equipment to provide effective electromagnetic interference (EMI) shielding. Pre localized CNF (CNF) powder will be mixed with Poly (vinylidene fluoride) (PVDF) and Ionic Liquid (IL) using solvent blending method to form a series of PVDF/CNF/IL composite films with different concentration of CNF and IL. Obtained composite films were characterized with Scanning Electron Microscopy (SEM) and Differential scanning calorimetry (DSC) for surface morphology and thermal analysis. Fabricated films were also examined for their mechanical properties. The dielectric properties of the film were measured with the help of impedance analyser. After this using dielectric properties of the films shielding effectiveness are calculated in the range of 100 KHz to 10 MHz. The fabricated film with composition of 60/10/30 exhibits the shielding effectiveness of 32 dB to 40 dB in entire frequency range and also has the elongation of 31%. The key advantage of obtained composite films is there light weight and flexibility can be used to shield small electronic equipment.

Flexible composite film for shielding of microwave radiation

Electromagnetic interference (EMI) disrupts the working of electronic devices and circuits. In this work materials have been exploited in the form of conducting polymer composite film to give effective EMI shielding properties. Pre localized Graphite(Gr) powder will be mixed with Poly vinylidene fluoride (PVDF) and Ionic Liquid (IL) using solvent blending method to form a series of PVDF/Gr/IL composite films with different concentration of Gr and IL. Obtained films were characterized with Scanning Electron Microscopy (SEM) and Differential scanning calorimetry (DSC) for surface morphology and thermal analysis. The dielectric properties of the film were measured through which shielding effectiveness of the film is calculated for both near field and far field region in the frequency range of 100 KHz to 10 MHz. The composition with 70/10/20 exhibits maximum shielding effectiveness of 35 dB, 120 dB and 40 dB for plane wave, electric field and magnetic field respectively. The fabricated films exhibit excellent EMI Shielding properties with extra advantage of low cost and flexibility.

Flexible multilayered films consisting of alternating nanofibrillated cellulose/Fe3O4 and carbon nanotube/polyethylene oxide layers for electromagnetic interference shielding

Along with the integration and miniaturization of modern electronics, electromagnetic radiation and heat accumulation have become the increasingly serious problem. However, it is still greatly challenging to achieve high electromagnetic interference (EMI) shielding effectiveness (SE) and thermal conductivity (TC) simultaneously in polymeric composite films. Herein, flexible and tough nanofibrillated cellulose/Fe3O4&carbon nanotube/Polyethylene oxide (NFC/Fe3O4&CNT/PEO) films featured with alternating multilayered structures were successfully prepared by a facile alternating vacuum-assisted filtration (AVF) method. The conductive CNT/PEO acted as the EMI shielding layer; the polymeric NFC/Fe3O4 played the role as supporting substrate and synergistically enhanced the EMI shielding performance. Thus, alternating multilayered NFC/Fe3O4&CNT/PEO films exhibited the high electrical conductivity of 3.9 × 103 S/m, excellent EMI SE of 30.3 dB, and thermal conductivity of 9.53 W m−1 K−1. In addition, NFC/Fe3O4&CNT/PEO films showed wonderful mechanical properties with a tensile strength of 36.03 MPa, a toughness of 2.98 MJ/m3, and an elongation at break of 19.1%, due to strong hydrogen bonding between NFC and PEO and hierarchical “zigzag” cracks. Interestingly, alternating multilayered structures could highly improve the toughness and ductility of composite films, in contrast to pure NFC. In the actual EMI shielding application measurement, NFC/Fe3O4&CNT/PEO films were proved to effectively block the electromagnetic wave transmission. This effort opens a creative avenue for designing and constructing flexible and tough composite films with both excellent EMI shielding performance and fascinating heat removal ability.

Assessment of physicomechanical properties of composite films based on a styrene-acrylic polymer, glycidyl ether, and a 3-aminopropyltriethoxysilane compatibilizer

The study concerns composite materials based on polymer mixtures of a styrene-acrylic polymer, glycidyl ether, and a 3-aminopropyltriethoxysilane (APTES) compatibilizer. The use of a silane-type compatibilizer improves the compatibility of the components and has been shown to significantly increase the degree of crosslinking of the composition components. In this work, the structural parameters of the polymer network of the composition components depending on the compatibilizer concentration were researched by the method of equilibrium swelling. The optimal concentration of the compatibilizer was found to maximize the degree of crosslinking with a minimal number of active chains. This fact proves that the crosslinking in the composition is complete and the molecule does not contain active sites that have not reacted with the compatibilizer. The swelling kinetics of the polymer composite films proves that with an increase in the degree of crosslinking, the swelling of the polymer films decreases. Polymer films with a low proportion of active chains practically do not swell after the crosslinking process.The article describes a possible mechanism of compatibilization involving 3-aminopropyltriethoxysilane as well as styrene-acrylic and glycidyl ether polymers. The 3-aminopropyltriethoxysilane compatibilizer has active functional groups that are located on opposite sides of the molecule; these are three active hydroxyl groups and one active amino group. Due to the presence of various functional groups, this compatibilizer can bind the polymers and thereby form strong polymer films.This gives grounds to assert that the control of the compatibilizer concentration and the degree of crosslinking of the composition components provide prospects for the creation of polymer films with high physical and mechanical characteristics due to the high interfacial adhesion of the components in the composition

Cyanopyridone doped PMMA films as UV and blue light filters: Preparation and characterization

Cyanopyridone-based conjugated small molecule (CP) doped poly(methyl 2-methylpropenoate) polymeric films were obtained using solvent-casting approach with various concentrations of CP loading ranging from 1 to 6 wt%. Further, structure and linear absorption properties of the prepared polymeric films were investigated in detail. Structural characterizations of polymeric films were carried out using XRD technique, where an amorphous hump was noticed which indicates the non-crystalline nature of examined polymeric composites. Spectral assessment of the films like absorbance and transmittance were made by using spectrophotometer in the wavelength (λ) region ranging from 200 to 1100 nm and followed by the determinations of absorption index (k), as well as optical energy band gap (Eg). Results revealed that the optical constants vary with the amount of CP loading and also, these polymeric composite films effectively blocks nearly 94 % of UV and blue light transmission and hence these films can be used in the UV and blue region filters.

Electromagnetic Interference Shielding Properties of BaCo2Fe16O27 Nanoplatelets and RGO Reinforced PVDF Polymer Composite Flexible Films

AbstractThe electromagnetic Interference (EMI) shielding effectiveness of W‐Type barium hexaferrite (BaCo2Fe16O27) and reduced graphene oxide (RGO) nanofillers reinforced poly(vinylidenefluoride) (PVDF) polymer composite films are reported. Two different amounts of BaCo2Fe16O27 (10 wt% and 30 wt%) nanofillers and fixed amount of RGO (10 wt%) are loaded in PVDF matrix by solvent casting in order to fabricate the multifunctional PVDF/RGO/BaCo2Fe16O27 composite films. The synthesized samples are investigated using various instruments including X‐ray diffraction (XRD), Fourier‐transform infrared spectroscopy (FTIR), Raman spectroscopy, high resolution scanning electron microscopy (HRSEM), energy dispersive X‐ray spectroscopy (EDX), X‐ray photoelectron spectroscopy (XPS) and vibrating sample magnetometer (VSM) analysis. The microwave properties of PVDF/RGO/BaCo2Fe16O27 composites are tested with vector network analyser (VNA) in 8–12 GHz frequency (X‐Band). The possible mechanism of EMI shielding is investigated from the analysis of complex permittivity and permeability.The resultant flexible films exhibit desirable EMI SE of 35.94 dB at 11.8 GHz for the 10 wt% of BaCo2Fe16O27 addition in PVDF composite for a very small thickness of 0.2 mm. The combination of high dielectric loss ( tanδε = 1.63) and magnetic loss (tanδμ = 0.26) contributes to high absorption of 29.85 dB (&gt;99% attenuation) dominated over reflection. Thus, the simple and cost‐effective fabrication of ultrathin and flexible PVDF/RGO/BaCo2Fe16O27 composite film with low filler content has a great potential as suppresser in electromagnetic fields.

Influence of nanostructured VO-acetylacetonate coordination system with 2-(pyridin-4-ylmethylene) hydrazine-1-carbothioamide in pseudocapacitance performance of p-type conductive polymer composite film

ABSTRACT In this work, first, VO-acetylacetonate coordination system with 2-(pyridin-4-ylmethylene) hydrazine-1-carbothioamide (VO(acac)2L) was synthesised via sonochemical routes. Then POAP/VO(acac)2L films were fabricated through electropolymerization of poly ortho aminophenol (POAP) in the presence of VO(acac)2L and used as the active electrode of an electrochemical supercapacitor (SC) with a significant electrochemical properties improvement. X-ray diffraction (XRD) and field emission scanning electron microscopy (FESEM) was applied to characterise the structural state of the prepared samples. Also, some electrochemical methods such as electrochemical impedance spectroscopy (EIS), cyclic voltammetry (CV), and galvanostatic charge–discharge (GCD) were carried out for the system performance investigation. This work may open an avenue to develop efficient and robust nanocomposite materials for an energy storage device in an acidic medium.

Design and synthesis of PVDF-cloisite-30B nanocomposite fibers for energy harvesting applications

Polymer nanofibers of PVDF/Cloisite-30B clay composites were synthesized by far field electrospinning technique. Taguchi's L9 orthogonal array was used to study the effect of process parameters in electrospinning. Different polymer composite films were prepared with various composition and process parameters. The best result obtained with highest β-phase crystallinity with 89.7% with average fiber diameter of 79 nm. Further piezoelectric property of nanofiber composite was measured by oscilloscope actuated through a mechanical cam driven by a D C motor at different speed 500, 1000 and 1500 rpm respectively. Grey relation analysis was performed to identify the most significant process parameters for preparation of uniform nanofibers. Grey relation grading for response parameters was ranked 1 for highest β-phase crystallinity among the studied composites. The PVDF composite sample with 3% cloisite-30B showed high instantaneous voltage of 4.4V with applied voltage of 22 kV and collector plate distance of 12 cm.

Structural Colors by Synergistic Birefringence and Surface Plasmon Resonance.

One-dimensional nanomaterials including cellulose nanocrystals (CNCs) and gold nanorods (GNRs) are widely used in optical materials due to their respective inherent features: birefringence with accompanying light retardation and surface plasmon resonance (SPR). Herein, we successfully combine these properties of both nanorods to generate synergistic and readily tunable structural colors in hybrid composite polymer films. CNCs and GNRs are embedded either in the same or in separate films after unidirectional alignment in dynamic hydrogels. By synergistically leveraging CNCs and GNRs with diverse amounts in hybrid films or stacked separate films, wide-ranging structural colors are obtained, far beyond those from films solely with aligned CNCs or GNRs. Higher GNR contents enhance light absorption at 520 nm with promoted magenta colors, while more CNCs affect the overall phase retardation with light absorption between 400 and 700 nm between crossed polarizers. Moreover, adjusting the angles between films solely with CNCs or GNRs via a stacking/rotating technique successively manipulates colors with flexible film combinations. By rotating the films with aligned GNRs (0-180°), light absorption can traverse from ∼500 to 650 nm. Thus, tuning the adjustable synergism of birefringence of CNCs and SPR of GNRs provides great potential for structural colors, which enlightens inspirations for designing functional optical materials.