Thermally activated shape memory behavior of melt‐mixed polyurethane/cellulose nanocrystal composites

Building blocks made from renewable sources attract increasing attention for the design of new polymer systems. Recently, in this particular context, cellulose nanocrystals (CNCs) have gained great interest in both academic research and industry, mainly on account of their ability to reinforce range of polymer matrices and afford nanocomposites with attractive mechanical properties. The limited thermal stability of conventionally produced cellulose nanocrystals (CNCs) has, however, so far limited the range of polymers that could be used as basis for melt‐processed CNC nanocomposites. We herein show that a commercially accessible nanocrystal source, a particular grade of microcrystalline cellulose (MCC), can easily be converted into thermally stable CNCs by ultrasonication in phosphoric acid. A scalable melt‐mixing process was used to produce nanocomposites of these CNCs with a thermoplastic polyurethane (TPU) elastomer. A significant improvement of the room temperature storage modulus from 40 MPa (neat polymer) to 120 MPa (10% w/w CNC) was observed. The introduction of CNCs not only increased the stiffness of the polymer matrix, but also improved the shape memory properties of the nanocomposite. © 2017 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2017 , 134, 45033.     

Poly(methyl methacrylate)‐grafted cellulose nanocrystals: One‐step synthesis,nanocomposite preparation,and characterization

Cellulose nanocrystals (CNCs) are ideal reinforcing agents for polymer nanocomposites because they are lightweight and nano‐sized with a large aspect ratio and high elastic modulus. To overcome the poor compatibility of hydrophilic CNCs in non‐polar composite matrices, we grafted poly(methyl methacrylate) (PMMA) from the surface of CNCs using an aqueous, one‐pot, free radical polymerization method with ceric ammonium nitrate as the initiator. The hybrid nanoparticles were characterized by CP/MAS NMR, X‐ray photoelectron spectroscopy, infrared spectroscopy, contact angle, thermogravimetric analysis, X‐ray diffraction, and atomic force microscopy. Spectroscopy demonstrates that 0.11 g/g (11 wt %) PMMA is grafted from the CNC surface, giving PMMA‐g‐CNCs, which are similar in size and crystallinity to unmodified CNCs but have an onset of thermal degradation 45 °C lower. Nanocomposites were prepared by compounding unmodified CNCs and PMMA‐g‐CNCs (0.0025–0.02 g/g (0.25–2 wt %) loading) with PMMA using melt mixing and wet ball milling. CNCs improved the performance of melt‐mixed nanocomposites at 0.02 g/g (2 wt %) loading compared to the PMMA control, while lower loadings of CNCs and all loadings of PMMA‐g‐CNCs did not. The difference in Young's modulus between unmodified CNC and polymer‐grafted CNC composites was generally insignificant. Overall, ball‐milled composites had inferior mechanical and rheological properties compared to melt‐mixed composites. Scanning electron microscopy showed aggregation in the samples with CNCs, but more pronounced aggregation with PMMA‐g‐CNCs. Despite improving interfacial compatibility between the nanoparticles and the matrix, the effect of PMMA‐g‐CNC aggregation and decreased thermal stability dominated the composite performance.     

Development and characterization of bionanocomposites based on poly(3‐hydroxybutyrate) and cellulose nanocrystals for packaging applications

Poly(3‐hydroxybutyrate) (PHB)‐based bionanocomposites were prepared using various percentages of cellulose nanocrystals (CNCs) by a solution casting method. CNCs were prepared from microcrystalline cellulose using sulfuric acid hydrolysis. The influence of CNCs on PHB properties was evaluated using differential scanning calorimetry, Fourier transform infrared spectroscopy, X‐ray diffraction, thermogravimetry and tensile testing. Vapor permeation and light transmission of the materials were also measured. Differential scanning calorimetric tests demonstrated that CNCs were effective PHB nucleation agents. Tensile strength and Young's modulus of PHB increased with increasing CNC concentration. Moreover, the PHB/CNC bionanocomposites exhibited reduced water vapor permeation compared to neat PHB and had better UV barrier properties than commodity polymers such as polypropylene. It was found that nanocomposites with 6 wt% of CNCs had the optimum balance among thermal, mechanical and barrier properties. © 2016 Society of Chemical Industry     

Melt processing of polyamide 12 and cellulose nanocrystals nanocomposites

The fabrication of nanocomposites of polyamide 12 (PA12) and cellulose nanocrystals (CNCs) isolated from cotton and tunicates is reported. Through a comparative study that involved solution‐cast (SC) and melt‐processed materials, it was shown that PA12/CNC nanocomposites can be prepared in a process that appears to be readily scalable to an industrial level. The results demonstrate that CNCs isolated from the biomass by phosphoric acid hydrolysis display both a sufficiently high thermal stability to permit melt processing with PA12, and a high compatibility with this polymer to allow the formation of nanocomposites in which the CNCs are well dispersed. Thus, PA12/CNC nanocomposites prepared by melt‐mixing the two components in a co‐rotating roller blade mixer and subsequent compression molding display mechanical properties that are comparable to those of SC reference materials. Young's modulus and maximum stress could be doubled in comparison to the neat PA12 by introduction of 10% (CNCs from tunicates) or 15% w/w (CNCs from cotton) CNCs. © 2015 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2015 , 132, 42752.     

Nanocomposites of PBAT and cellulose nanocrystals modified by in situ polymerization and melt extrusion

Cellulose nanocrystals (CNC) were successfully grafted with a low molecular weight poly(butylene glutarate) through an in situ polymerization procedure. The grafting treatment decreased the CNC hydrophilic character and increased the onset of their thermal degradation by approximately 20°C, thus increasing the possibilities of CNC application. Composites of grafted and nongrafted CNC with a poly(butylene‐adipate‐co‐terephthalate) (PBAT) matrix were prepared by melt extrusion. The CNC addition led to an increase of 50% of the tensile elastic modulus of the PBAT. In addition, dynamic mechanical thermal analysis showed that the composite with CNC retained its high modulus even at temperatures far above the glass transition temperature of PBAT. At 60°C the storage modulus of the composite with CNC was approximately 200% higher than that of the pure PBAT. Thus, in this work, nanocomposites of improved properties were obtained through a combination of in situ polymerization and melt extrusion. POLYM. ENG. SCI., 56:1339–1348, 2016. © 2016 Society of Plastics Engineers     

Synthesis and characterization of biodegradable aliphatic–aromatic nanocomposites fabricated using maleic acid‐grafted poly[(butylene adipate)‐co‐terephthalate] and organically modified layered zinc phenylphosphonate

A new series of biodegradable aliphatic–aromatic nanocomposites containing maleic acid‐grafted poly[(butylene adipate)‐co‐terephthalate] (g‐PBAT) and organically modified layered zinc phenylphosphonate (m‐PPZn) were successfully synthesized through transesterification and polycondensation processes with covalent linkages between the polymeric and inorganic materials. Fourier transform infrared and ¹³C NMR spectra demonstrate the successful grafting of maleic acid to PBAT. The morphology of g‐PBAT/m‐PPZn nanocomposites was investigated using wide‐angle X‐ray diffraction and transmission electron microscopy. Results showed that the stacking layers of m‐PPZn were distributed and intercalated into the g‐PBAT polymer matrix. The incorporation of m‐PPZn into the g‐PBAT matrix significantly enhanced the storage modulus at ?70 °C as compared to that of neat g‐PBAT. A reduction in thermal stability was observed for all g‐PBAT/m‐PPZn systems, which is probably due to the lower thermal stability of m‐PPZn. The biodegradation of neat g‐PBAT copolymers and g‐PBAT/m‐PPZn nanocomposites was investigated using lipase from Pseudomonas sp. The degradation rates of neat g‐PBAT copolymers decrease in the order g‐PBAT‐80 > g‐PBAT‐50 > g‐PBAT‐20. The faster degradation rate of g‐PBAT‐80 is a result of the higher content of adipate acid units and the chain flexibility of the polymer backbone. Furthermore, the weight loss increases as the loading of m‐PPZn increases, indicating that the presence of m‐PPZn improves the degradation of the g‐PBAT copolymers. This result might be accounted for by the lower degree of crystallinity for g‐PBAT/m‐PPZn nanocomposites. © 2019 Society of Chemical Industry     

Optimizing 3D printing performance of acrylonitrile‐butadiene‐styrene composites with cellulose nanocrystals/silica nanohybrids

The preparation of 3D printed products with excellent comprehensive performance is still receiving much attention. Cellulose, the most abundant and green natural polymer, was used in this study to fabricate polymeric composites used for 3D printing. Specifically, novel cellulose nanocrystals/silica nanohybrids (CSNs) were synthesized via the sol–gel method using cellulose nanocrystals (CNCs) obtained by hydrolysis of sulfuric acid as raw materials, and the thermostability was significantly improved due to the adsorption of silica (SiO₂) on the surface of the CNCs via hydrogen bonding and covalent bonds. Subsequently, the CSNs were used in fused deposition modeling (FDM) with acrylonitrile‐butadiene‐styrene (ABS) as the matrix. Unlike ABS/CNC product which shows obvious yellowing, the ABS/CSN product shows a smooth undefiled surface, demonstrating their excellent applicability to high temperature FDM molding. Further, the effect of different silane coupling agents on the mechanical properties was compared and organically modified CSNs (oCSNs) were prepared using KH570 to optimize the dispersion of the filler and the interaction with the matrix. Satisfactorily, the addition of organically modified oCSNs not only does not degrade the fluidity but it also eliminates the warpage of FDM products and improves both layer adhesion and mechanical properties. This study provides a pioneering strategy for the thermal processing applications of CNCs and the modification of FDM products. © 2019 Society of Chemical Industry     

Formulation and characterization of compatibilized poly(lactic acid)‐based blends and their nanocomposites with silver‐loaded kaolinite

Biodegradable polymer nanocomposites have been developed in this study as materials for use in the packaging of moisture‐sensitive products. Poly(lactic acid) (PLA) was the main component of the nanocomposites with poly(butylene adipate‐co‐terephthalate) (PBAT) as flexibility enhancer. Tetrabutyl titanate was also added as a compatibilizer to enhance the interfacial affinity between PLA and PBAT by inducing the formation of some PLA/PBAT via transesterification during the melt blending process, thereby improving the mechanical properties of the blends. Silver‐loaded kaolinite synthesized via chemical reduction was also incorporated into the compatibilized blends for further property improvement. Herein, we report a novel biodegradable quaternary nanocomposite system with intercalated‐exfoliated clay dispersion that was uniquely achieved by increasing the interlamellar space between kaolinite layers through silver nanoparticle insertion. The resultant nanocomposites containing as little as 4 phr modified clay reduced the elongation at break from 213.0 ± 5.85% to 53.8 ± 1.81%, enhanced thermal stability (initial decomposition temperature increased from 378 °C to 399 °C) and exhibited a water vapor permeability reduction of 41.85%. On the basis of these properties, the developed nanocomposites are considered to be promising candidates for use in bio‐packaging applications to replace non‐biodegradable and petro‐based plastics. © 2014 Society of Chemical Industry     

Melt extruded nanocomposites of polybutylene adipate‐co‐terephthalate (PBAT) with phenylbutyl isocyanate modified cellulose nanocrystals

Traditional commodity polymers are widely used in several disposable or short‐life items and take hundreds of years to decompose in nature. These polymers could be replaced in several uses by biodegradable polymers, like polybutylene adipate‐co‐terephthalate (PBAT) studied in this work. For this, nonetheless, it is necessary to improve some of the PBAT properties, like mechanical resistance and barrier properties. In this work, cellulose nanocrystals (CNC) were incorporated in PBAT with this intention, through melt extrusion. Aiming to avoid CNC aggregation during the drying and extrusion process, a CNC chemical modification with phenylbutyl isocyanate was done. It was possible to obtain PBAT‐CNC melt extruded composites with an elastic modulus 55% higher and water vapor permeability 63% lower than the values of the pure polymer, without compromising PBAT biodegradation. Therefore, the composites prepared with these enhanced properties have great potential as substitutes for traditional commodity polymers. © 2016 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2016 , 133, 43678.     

Starch‐based biocomposite films reinforced with cellulose nanocrystals from garlic stalks

The study was conducted to reinforce starch‐based biocomposite films using cellulose nanocrystals (CNCs) from garlic stalks. An average yield of 4.6% by mass based from air‐dried garlic stalks was obtained through alkali delignification, acid hydrolysis and sonication. The isolated CNCs are spherical and have an average diameter of 35 nm and crystallinity of 62%. Fourier transform infrared spectra correspond to the structure of cellulose, but some absorption bands corresponding to hemicelluloses were also noticed. Starch‐based biocomposite films with varying amount of the isolated CNCs as reinforcing filler were prepared by solution casting and evaporation method. Scanning electron micrographs of the films showed homogeneous dispersion of CNC in the starch matrix. Improvement in tensile strength and modulus was at maximum when the starch to CNC ratio is 100:5. The thermal stability of the films, on the other hand, decreased with the addition of CNC. Finally, CNC‐reinforced films had lower moisture uptake than nonreinforced films. POLYM. COMPOS. 34:1325–1332, 2013. © 2013 Society of Plastics Engineers     

Polyamide 6 nanocomposites incorporating cellulose nanocrystals prepared by In situ ring‐opening polymerization: Viscoelasticity,creep behavior,and melt rheological properties

The creep behavior and solid and melt linear viscoelasticity of novel polyamide 6 (PA6) nanocomposites reinforced with cellulose nanocrystals (CNCs) prepared via in situ anionic ring‐opening polymerization (ROP) were investigated to accelerate research efforts to develop new polymeric materials with improved properties for lightweight, load‐bearing applications. The obtained results showed that incorporation of relatively small amounts of ≤ 2wt% CNCs into the PA6 thermoplastic matrix gave nanocomposite samples with significantly enhanced creep and viscoelastic materials functions of the PA6 as indicated by lower creep strain, lower creep compliance, improved elastic recovery after removal of load, and reduced Arrhenius activation energies for time‐dependent viscoplastic flow. The obtained results were analyzed and interpreted by theoretical equations for predicting the viscoelasticity and creep behavior of polymeric systems. The melt rheological properties showed enhanced melt strength and elasticity. The formation of a percolated network structure of CNC was revealed by morphological observations that were consistent with the dynamic structure break‐up and reformation rheological experiments. The stiffness, rigidity of the CNCs along with their special ROP‐facilitated intrinsic strong chemical interactions with the PA6 matrix is believed to be responsible for the observed superior creep and viscoelastic materials functions even with very little CNC concentration. POLYM. ENG. SCI. 56:1045–1060, 2016. © 2016 Society of Plastics Engineers     

Enhanced thermal stability of biomedical thermoplastic polyurethane with the addition of cellulose nanocrystals

Freeze‐dried cellulose nanocrystals (CNCs) were dispersed in the thermoplastic polyurethane [Pellethane 2363‐55D (P55D)] by a solvent casting method to fabricate CNC‐reinforced nanocomposites. This study demonstrated that the addition of small amounts (1–5 wt %) of CNCs to P55D increased the thermal degradation temperature while maintaining a similar stiffness, strength, and elongation of the neat P55D. CNC additions to P55D did not alter the glass‐transition temperature, but the onset decomposition temperature was shifted from 286 to 327°C when 1 wt % CNCs was dispersed in the matrix. The higher onset decomposition temperature was attributed to the formation of hydrogen bonds between the hydroxyl groups on the CNC surface and urethane groups in the hard block of P55D. The ultimate tensile strength and strain to failure (ε_f) of the nanocomposites were minimally affected by additions up to 5 wt % CNCs, whereas the elastic modulus was increased by about 70%. The observation that ε_f was unchanged with the addition of up to 5 wt % CNCs suggested that the flow/sliding of the hard blocks and chains were not hindered by the presence of the CNCs during plastic deformation. The ramifications of this study was that CNC additions resulted in wider processing temperatures of P55D for various biomedical devices while maintaining a similar stiffness, strength, and elongation. © 2015 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2015 , 132, 41970.     

Analyzing three‐dimensional structure and geometrical shape of individual cellulose nanocrystal from switchgrass

The three‐dimensional morphology, size distribution, and structure of individual cellulose nanocrystals (CNCs) isolated from switchgrass (Panicumvirgatum L), a representative raw biomass material, were investigated in this research. Width and height evolutions along the individual CNC longitudinal direction were statistically and quantitatively characterized using transmission electron microscopy (TEM) and atomic force microscopy (AFM). Lognormal distribution was identified as the most likely for cellulose nanocrystals’ size distribution. Height and width dimensions were shown to decrease toward the ends from the midpoint of individual CNCs, implying a spindle shape. The observed rough surfaces of CNCs were explainable as the results of acid etching of the subcrystalline and disordered region located at the surface. X‐ray diffraction analysis of crystallite size accompanied with TEM and AFM measurements revealed that the cross‐sectional dimensions of individual switchgrass CNC were either rectangularly or elliptically shaped, with an approximately 3–5 nm lateral element length range. POLYM. COMPOS., 38:2368–2377, 2017. © 2015 Society of Plastics Engineers     

Nanocomposites of poly(propylene carbonate) reinforced with cellulose nanocrystals via sol‐gel process

Cellulose nanocrystals (CNCs) organogels were first produced from aqueous dispersion through solvent exchange of CNCs to acetone via a simple sol‐gel process. After mixing the organogels with poly(propylene carbonate) (PPC) in dimethylformamide followed by solution casting, green nanocomposites were obtained with CNCs well dispersed in PPC polymer matrix which was confirmed by scanning electron microscopy observations. Differential scanning calorimeter analysis revealed that glass transition temperature of the nanocomposites was slightly increased from 34.0 to 37.4°C. Tensile tests indicated that both yield strength and Young's modulus of CNCs/PPC nanocomposites were doubled by adding 10 wt % CNCs. However, poor thermal stability of PPC occurred after incorporating with CNCs due to the thermo‐sensitive sulfate groups located on the surface of CNCs. Furthermore, PPC became more hydrophilic because of the inclusion of CNCs according to the water contact angle measurement. The enhanced mechanical and hydrophilic properties, coupled with the inherent superior biocompatibility and degradability, offered CNCs/PPC composites potential application in biomedical fields. © 2014 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2014 , 131, 40832.     

Nanoclay‐reinforced poly(butylene adipate‐co‐terephthalate) biocomposites for packaging applications

Increasing generation and inadequate disposal of waste progressively compromise our environment. Solutions are proposed by the development of biodegradable polymers, that is, for short‐term applications like packaging. The present study focuses on the design and characterization of biodegradable poly(butylene adipate‐co‐terephthalate) (PBAT) nanocomposites reinforced by different types of nanoclays. The addition of natural and modified montmorillonite and bentonite to PBAT by melt mixing enhances slightly the thermal stability and increases the crystallization temperature, independently of the fillers' dispersion state. By contrast, storage modulus in dynamic mechanical analysis is increased when adding nanoclay, and improvement is higher for well‐dispersed organomodified fillers. Dispersion states and morphology of the nanocomposites are studied by X‐ray diffraction as well as scanning and transmission electron microscopy. PBAT‐based composites with modified bentonite reveal to show the best performance at room temperature (which is the temperature of interest for potential packaging applications) in comparison with the other investigated nanocomposites.POLYM. COMPOS., 33:2022–2028, 2012. © 2012 Society of Plastics Engineers     

Preparation and mechanical properties of green epoxy nanocomposites with cellulose nanocrystals

Epoxy resin is widely used to make composites, electronic and electric parts, adhesives, and coating materials because it has excellent thermal, electrical, and mechanical properties. Using natural materials in making epoxy composites and nanocomposites would make the final products greener. Therefore, in this study, epoxidized soybean oil (ESO) and cellulose nanocrystals (CNCs) were used to make green epoxy nanocomposites. ESO was prepared by epoxidation of soybean oil with peroxyacetic acid and it was confirmed by Fourier transform infrared spectroscopy. The ESO was mixed with diglycidyl ether of bisphenol A at different weight ratios (10%–50%) and the stoichiometric amount of ethylene diamine was used for curing. CNC content in the nanocomposites was changed from 0.125 to 1 phr. Mechanical properties of the epoxy samples and the nanocomposites were investigated by universal testing machine and izod impact tester. The epoxy sample showed best mechanical properties at ESO 30%. The nanocomposite with CNC 0.25 phr showed best mechanical properties. Fracture surfaces of the epoxy sample and the nanocomposites were investigated by scanning electronic microscope. POLYM. ENG. SCI., 60:439–445, 2020. © 2019 Society of Plastics Engineers     

Surface modification and antimicrobial properties of cellulose nanocrystals

A novel and simple surface modification of cellulose nanocrystals (CNC) was performed by chloroacetylation and subsequent reaction with tertiary amines to form quaternary ammonium modified CNCs. The acetylation of CNC and quaternary ammonium modified CNCs was confirmed using IR spectroscopy and solid state NMR spectroscopy. The ¹³C NMR spectrum of quaternary ammonium modified CNC showed several additional resonances ranging from 14.5 ppm to 58.0 ppm compared to ¹³C NMR spectrum of pure CNC, suggesting that alkyl chains have been added to the pure CNC. The disc diffusion method was used to evaluate the antimicrobial properties of quaternary ammonium modified CNCs. It was found that modified CNCs with alkyl chain longer than ten carbons are effective antimicrobial agents against Staphylococcus aureus and E. coli bacteria. These CNCs can be chemically modified to tailor the properties to improve dispersion in the polymer matrix. This will expand the application of CNC as a reinforcing material. © 2017 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2017 , 134, 44789.     

Preparation,crystallization, and properties of biodegradable poly(butylene adipate‐co‐terephthalate)/organomodified montmorillonite nanocomposites

Intercalated and exfoliated nanocomposites of biodegradable poly(butylene adipate‐co‐terephthalate) (PBAT) and Cloisite 30B (C30B) were fabricated by a solution‐casting method to study the effects of the clay loading on the crystallization behavior, thermal stability, and dynamic mechanical properties of PBAT in PBAT/C30B nanocomposites. X‐ray diffraction and transmission electron microscopy results indicated the formation of exfoliated nanocomposites at low clay loadings (<5 wt %) and a mixture of exfoliated and intercalated nanocomposites with a clay content of 8 wt % throughout the PBAT matrix. Nonisothermal melt crystallization studies indicated that C30B enhanced the crystallization of PBAT, apparently because of a heterogeneous nucleation effect. Moreover, an attempt was made to quantitatively study the influence of the presence of C30B and its contents on the nucleation activity of PBAT in the PBAT/C30B nanocomposites. The thermal stability of PBAT decreased slightly in the nanocomposites. However, the storage modulus of PBAT apparently increased with the C30B loading increasing in the PBAT/C30B nanocomposites. © 2010 Wiley Periodicals, Inc. J Appl Polym Sci, 2011     

Morphology and properties tuning of PLA/cellulose nanocrystals bio-nanocomposites by means of reactive functionalization and blending with PVAc

A novel method for the preparation of PLA bio-nanocomposites containing cellulose nanocrystals (CNCs) is reported. In order to enhance interfacial adhesion and dispersion of nanocrystals into PLA matrix, functionalization of PLA and CNCs by radical grafting of glycidyl methacrylate (GMA) and pre-dispersion of CNCs in poly (vinyl acetate) (PVAc) emulsion were applied. Morphologies, thermal and mechanical properties of nanocomposites for CNCs content of 1–6 wt.% were examined. Addition of functionalized components (PLA-GMA, CNC-GMA) and/or PVAc dispersed CNCs both improved the phase distribution of nanofiller and tensile properties, compared to the binary PLA/CNC nanocomposites. Thermal analyses demonstrated that glass transition, melting temperature and crystallinity of PLA were affected by the PVAc amount. Nanocomposites with PVAc dispersed CNCs exhibited higher thermal resistance than other composites. The filler effectiveness (CFE) was evaluated for all samples on the basis of storage modulus values: CNC-GMA and PVAc dispersed CNCs (3 wt. %) resulted the most effective fillers.     

Functionally Graded Polyurethane/Cellulose Nanocrystal Composites

The preparation and investigation of functionally graded polymer nanocomposites, which have a concentration gradient of cellulose nanocrystals (CNCs) along one direction, is reported here. As a test bed, a series of nanocomposites consisting of a thermoplastic polyurethane (PU) and 0–15% w/w CNCs is prepared via solvent casting and the mechanical properties of films of these materials are characterized by dynamic mechanical analyses and tensile tests. The formation of graded materials is accomplished by lamination of films with varying CNC content. The processing conditions are optimized to achieve intimate fusion of the individual layers. The elimination of internal interfaces is evidenced by an elongation at break of up to 500%. In order to explore potential applications of graded PU/CNC nanocomposites, structure‐dependent actuation in response to water is demonstrated in a bioinspired architecture. In addition, the damping behavior of cylindrical shaped composites is investigated by way of compression tests. The results show that functionally graded PU/CNC composites show good damping behavior over a much larger range of forces than the neat PU or the homogeneous nanocomposites.