Comparison of natural halloysite with synthetic carbon nanotubes in poly(lactic acid) based composites

The objective of this study is to compare the mechanical properties, structure and degradability of the nanocomposites prepared with tubular nanofillers, halloysite (HNT) and carbon nanotube (CNT) in poly(lactic acid) (PLA), and thermoplastic polyurethane (TPU) toughened PLA (T‐PLA) matrices. In the PLA matrix, CNT increased, whereas HNT decreased the tensile strength with increasing filler content. Also, the elongation at break and impact strength decreased with increasing CNT content, but these properties were relatively unchanged with increasing HNT content. However, when (TPU) was used as an impact modifier‐compatibilizer, addition of HNT further increased the impact strength and the elongation at break of the matrix, since short and straight HNT fibers were pulled out from the extensible, toughened matrix. The long and curvy CNT fillers always caused brittle fracture and affected the impact strength and elongation at break in a negative manner as the CNT content was increased. Both types of fillers did not significantly influence the degradation of PLA or toughened PLA matrices. POLYM. COMPOS., 38:2337–2346, 2017. © 2015 Society of Plastics Engineers     

Reactive compatibilization of PLA/TPU blends with a diisocyanate

This study focuses on the compatibilization of poly(lactic acid) (PLA)/thermoplastic polyurethane (TPU) blends by using 1,4 phenylene diisocyanate (PDI) for the first time, as the compatibilizer. Because of the potential interactions of diisocyanates with ? OH/? COOH, they are useful for reactive processing of PLA/TPU blends in the melt processing. To have insight on the reactively compatibilized structure of PLA/TPU blends, phase morphologies are observed by means of scanning electron microscopy. The mechanical, thermal, and rheological responses of the blends are investigated. The observations are that the brittle behavior of PLA changes to ductile with the addition of TPUs. The addition of PDI improves the tensile properties of the blends. The compatibilization action of PDI is monitored with DMA and rheological experiments. Cross‐over in the G′ and G″ curves of compatibilized blends indicates the relaxation of branches formed in the presence of PDI. The dispersed phase size of TPU decreases in PLA in the presence of PDI due to the improved compatibility. © 2013 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2014 , 131, 40251.     

Influence of the morphology and viscoelasticity on the thermomechanical properties of poly(lactic acid)/thermoplastic polyurethane blends compatibilized with ethylene-ester copolymer

Viscoelastic, interfacial properties, and morphological data were employed to predict the thermal and mechanical properties of compatibilized poly(lactic acid) (PLA)/thermoplastic polyurethane (TPU) blends. The combination of interfacial thickness measured by contact angle and entanglement density determined by dynamical mechanical analysis analyze data was employed to evaluate the mechanical behavior of PLA/TPU blends with and without ethylene-butyl acrylate-glycidyl methacrylate (EBG) compatibilization agent. The PLA/TPU blend (70/30 wt %) was prepared in a Haake internal mixer at 190 °C and compatibilized with different contents of EBG. The evaluation of the interfacial properties revealed an increase in the interfacial layer thickness of the PLA/TPU blend with EBG. The scanning electronic microscopy images showed a drastic reduction in the size of the dispersed phase by increasing the compatibilizer agent EBG content in the blend. The compatibilization of the PLA/TPU blends improved both the Izod impact strength and yield stress by 38 and 33%, respectively, in comparison with neat PLA/TPU blend. The addition of EBG into PLA/TPU blends significantly increased the entanglement density and the PLA toughening but resulted in a decrease of PLA deformation at break. The PLA and TPU glass transitions were affected by the EBG, suggesting that the PLA and TPU domains were partially miscible. © 2020 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2020 , 137, 48926.     

Dynamic rheological and morphological study of the compatibility of thermoplastic polyurethane/ethylene–octene copolymer blends

Two grafted ethylene–octene copolymers [POEs; i.e., POE‐g‐maleic anhydried (MAH) and aminated POE (denoted by POE‐g‐NH₂) were used as compatibilizers in immiscible blends of thermoplastic polyurethane (TPU) and POE. The effects of the compatibilizers on the dynamic rheological properties and morphologies of the TPU/POE blends were investigated. The characteristic rheological behaviors of the blends indicated that the strong interactions between the two phases were due to the compatibilization. Microstructural observation confirmed that the compatibilizers were located at the interface in the blends and formed a stable interfacial layer and smaller dispersed phase particle size. Compared with POE‐g‐MAH, POE‐g‐NH₂ exhibited a better compatibilization effect in the TPU/POE blends. © 2008 Wiley Periodicals, Inc. J Appl Polym Sci, 2008     

Mechanical and thermal properties of thermoplastic polyurethane‐toughened polylactide‐based nanocomposites

The crystallinity and mechanical and thermal properties of polylactide (PLA)‐based biodegradable‐engineered plastic nanocomposites were determined. The nanocomposites were composed of thermoplastic polyurethane (TPU)‐toughened PLA, Talcum (Talc) and organic modified clay (montmorillonite; OMC). The tensile and flexural tests showed that PLA blended with 10 wt% TPU, 4 wt% Talc powder and 2 wt% OMC had the highest modulus and strength without a loss of elongation. The heat distortion temperature (HDT) tests demonstrated that the thermally treated PLA‐based nanocomposites had an HDT of nearly double the HDT for untreated specimens. An analysis of the polymer using scanning electron microscopy demonstrated that the incorporation of inorganic fillers altered the heterogeneous morphology of the PLA/TPU blend. This study investigated the feasibility of using PLA‐based nanocomposites for practical use, including applications in the automotive and furniture industries. POLYM. COMPOS., 35:1744–1757, 2014. © 2013 Society of Plastics Engineers     

The study of morphology,thermal and thermo‐mechanical properties of compatibilized TPU/SAN blends

The compatibilizing efficiency of three different compatibilizers in thermoplastic polyurethane/styrene‐co‐acrylonitrile (TPU/SAN) blends was investigated after their incorporation via melt‐mixing. The compatibilizers studied were poly‐ε‐caprolactone (PCL), a mixture of polystyrene‐block‐polycaprolactone (PS‐b‐PCL) and polystyrene‐block‐poly(methyl methacrylate) (PS‐b‐PMMA), and a mixture of polyisoprene‐block‐polycaprolactone (PI‐b‐PCL) and polybutadiene‐block‐poly(methyl methacrylate) (PB‐b‐PMMA). All compatibilizers were synthesized by living anionic polymerization. Investigations of thermal and thermo‐mechanical properties performed by differential scanning calorimetry (DSC) and dynamic mechanical thermal analysis (DTMA), respectively, were systematically classified into two groups, i.e. blends of TPU or SAN with 20 wt% of different compatibilizers (so‐called limit conditions) and TPU/SAN 25/75 blends with 5 wt% of different compatibilizers. In order to determine the compatibilizer's location, morphology of TPU/SAN 25/75 blends was studied with transmission electron microscopy (TEM). Different compatibilization activity was found for different systems. Blends compatibilized with PCL showed superior properties over the other blends. Polym. Eng. Sci. 44:838–852, 2004. © 2004 Society of Plastics Engineers.     

Effects of thermoplastic polyurethane on the properties of poly(lactic acid)/organo‐montmorillonite nanocomposites based on novel vane extruder

Polylactic acid (PLA)/organo‐montmorillonite (OMMT) nanocomposites toughened with thermoplastic polyurethane (TPU) were prepared by melt‐compounding on a novel vane extruder (VE), which generates global dynamic elongational flow. In this work, the mechanical properties of the PLA/TPU/OMMT nanocomposites were evaluated by tensile, flexural, and tensile tests. The wide‐angle X‐ray diffraction and transmission electron microscopy results show that PLA/TPU/OMMT nanocomposites had clear intercalation and/or exfoliation structures. Moreover, the particles morphology of nanocomposites with the addition of TPU was investigated using high‐resolution scanning electronic microscopy. The results indicate that the spherical TPU particles dispersed in the PLA matrix, and the uniformity decreased with increasing TPU content (≤30%). Interestingly, there existed abundant filaments among amount of TPU droplets in composites with 30 and 40 wt% TPU. Furthermore, the thermal properties of the nanocomposites were examined with differential scanning calorimeter and dynamic mechanical analysis. The elongation at break and impact strength of the PLA/OMMT nanocomposites were increased significantly after addition of TPU. Specially, Elongation at break increased by 30 times, and notched impact strength improved 15 times when TPU loading was 40 wt%, compared with the neat PLA. Overall, the modified PLA nanocomposites can have greater application as a biodegradable material with enhanced mechanical properties. POLYM. ENG. SCI., 54:2292–2300, 2014. © 2013 Society of Plastics Engineers     

Morphologies and mechanical properties of polylactide/thermoplastic polyurethane elastomer blends

To explore a potential method for improving the toughness of a polylactide (PLA), we used a thermoplastic polyurethane (TPU) elastomer with a high strength and toughness and biocompatibility to prepare PLA/TPU blends suitable for a wide range of applications of PLA as general‐purpose plastics. The structure and properties of the PLA/TPU blends were studied in terms of the mechanical and morphological properties. The results indicate that an obvious yield and neck formation was observed for the PLA/TPU blends; this indicated the transition of PLA from brittle fracture to ductile fracture. The elongation at break and notched impact strength for the PLA/20 wt %TPU blend reached 350% and 25 KJ/m², respectively, without an obvious drop in the tensile strength. The blends were partially miscible systems because of the hydrogen bonding between the molecules of PLA and TPU. Spherical particles of TPU dispersed homogeneously in the PLA matrix, and the fracture surface presented much roughness. With increasing TPU content, the blends exhibited increasing tough failure. The J‐integral value of the PLA/TPU blend was much higher than that of the neat PLA; this indicated that the toughened blends had increasing crack initiation resistance and crack propagation resistance. © 2010 Wiley Periodicals, Inc. J Appl Polym Sci, 2011     

Investigation of structure and mechanical properties of toughened poly(l‐lactide)/thermoplastic poly(ester urethane) blends

In this study, poly(l ‐lactide) (PLA) is melt‐blended with thermoplastic polyurethane (TPU) to modify the brittleness of PLA. An aliphatic ester‐based TPU was selected in order to have an ester sensitivity for degradation and an inherent biocompatibility. Using this compatible TPU, there was no need to apply problematic compatibilizers, so the main positive properties of PLA such as biocompatibility and degradability were not challenged. The detected microstructure of PLA/TPU blends showed that when the TPU content was lower than 25 wt %, the structure appeared as sea‐islands, but when the TPU content was increased, the morphology was converted to a cocontinuous microstructure. A higher interfacial surface area in the blend with 25 wt % TPU (PLA25) resulted in a higher toughness and abrasion resistance. The various analyses confirmed interactions and successful coupling of two phases and confirmed that melt‐blending of PLA with the aliphatic ester‐based TPU is a convenient, cost‐effective, and efficient method to conquer the brittleness of PLA. The prepared blends are general‐purpose plastics, but PLA25 showed an optimum mechanical strength, toughness, and biocompatibility suitable for a wide range of applications. © 2015 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2016 , 133, 43104.     

The morphology,properties, and shape memory behavior of polylactic acid/thermoplastic polyurethane blends

Biodegradable polylactic acid (PLA) was compounded with thermoplastic polyurethane (TPU) by twin‐screw extrusion at weight ratios of 90/10, 80/20, 70/30, and 60/40. The blends were investigated based on their phase morphology, thermal and mechanical properties, and shape memory properties. The tensile results showed that PLA was successfully toughened by TPU. When the TPU content was 40%, the elongation‐at‐break increased to 400%. The SEM morphology showed that TPU was dispersed uniformly in the PLA matrix; DMA and DSC results indicated that the two polymers were immiscible. Most interestingly, it was found that the blends exhibited a shape memory behavior and, unlike most of the existing shape memory polymers (SMPs), the PLA/TPU blends could be deformed at room temperature without an extra heating and cooling step. During the deformation process, TPU acted as a toughening agent that prevented the PLA/TPU blends from breaking; thus, the temporary shape could be kept and internal stress was stored in the blends. Upon heating to above the glass transition temperature of PLA (about 60°C), the deformed parts regained their original shapes quickly along with the release of the stress. POLYM. ENG. SCI., 55:70–80, 2015. © 2014 Society of Plastics Engineers     

Studies on electrical properties of nanoclay filled thermoplastic polyurethane/polypropylene blends

The electrical properties of ester/ether‐based thermoplastic polyurethane (TPU) and polypropylene (PP) blends are presented in this article. Special attention has been paid to analyze the effect of blend ratio, compatibilization, and effect of nanoclay on the electrical properties of TPU/PP blends. The electrical properties measured were dielectric constant (ε′), volume resistivity (ρ_υ), loss factor (ε″), and dissipation factor (tan δ). Addition of PP into TPU increases the volume resistivity and reduces the dissipation and loss factor due to the decrease in the overall polarity of the system. Further addition of compatibilizer and nanoclay to this system reduced the dissipation factor and loss factor with increased volume resistivity. Compared with the ether‐TPU based blend nanocomposites, the ester‐TPU blends show better compatibility as confirmed by analysis. POLYM. COMPOS., 35:1671–1682, 2014. © 2013 Society of Plastics Engineers     

Elongational rheology of biodegradable poly(lactic acid)/poly[(butylene succinate)‐co‐adipate] binary blends and poly(lactic acid)/poly[(butylene succinate)‐co‐adipate]/clay ternary nanocomposites

A series of blends based on poly(lactic acid) (PLA) and poly[(butylene succinate)‐co‐adipate] (PBSA) as well as their nanocomposites with nanoclay (PLA/PBSA/Clay ternary nanocomposites) were prepared using the twin‐screw extruder. The blends were prepared for PBSA contents ranging from 25 to 75 wt % and their corresponding nanocomposites were prepared at a single‐clay concentration. The morphology and structure of the blends and the nanocomposites were examined using field emission scanning electron microscopy, transmission electron microscopy, and X‐ray diffraction. Rheological properties (dynamic oscillatory shear measurements and elongational viscosities) of the blends, nanocomposites, and pure components were studied in detail. The strain hardening intensity of different blends and nanocomposites was compared with the behavior of the pure components. Strong strain hardening behavior was observed for blends composed of 50 wt % and higher PBSA content. However, the effect of PBSA content on the elongational viscosity was less pronounced in PLA/PBSA/Clay ternary nanocomposites. © 2012 Wiley Periodicals, Inc. J. Appl. Polym. Sci., 2013     

Influence of phthalic anhydride and bioxazoline on the mechanical and morphological properties of biodegradable poly(lactic acid)/poly[(butylene adipate)‐co‐terephthalate] blends

Poly(lactic acid) (PLA)/poly[(butylene adipate)‐co‐terephthalate] (PBAT) blends were fabricated by melt blending, with 2,2′‐(1,3‐phenylene)bis(2‐oxazoline) (BOZ) and phthalic anhydride (PA) used as compatibilizers. It was found that a small amount of BOZ or PA greatly increased the elongation at break of the PLA/PBAT blends without sacrificing their high tensile strength. Scanning electron microscopy results revealed that the PBAT particles became finer and were uniformly dispersed in the matrix when the compatibilizers were incorporated, which indicated that the interfacial bonding and compatibilization between PLA and PBAT were improved in the presence of the compatibilizers. Compared with PLA/PBAT blends, the molecular weight of PLA/PBAT/PA/BOZ blends was increased due to chain‐extending reactions. Differential scanning calorimetry results suggested PBAT decreased the crystallization rate and crystallinity of PLA in the blends. Moreover, the glass transition temperature of PBAT was further decreased when the compatibilizers were used. © 2013 Society of Chemical Industry     

Reactive modification and compatibilization of poly(lactide) and poly(butylene adipate‐co‐terephthalate) blends with epoxy functionalized‐poly(lactide) for blown film applications

Biodegradable blown films comprising of poly(lactide) (PLA) and poly(butylene adipate‐co‐terephthalate) (PBAT) were produced using epoxy functionalized‐poly(lactide) (EF‐PLA) reactive modifiers for rheological enhancement and compatibilization. The epoxy groups on the EF‐PLA modifiers react with PBAT forming an in situ copolymer that localizes at the blend interphase resulting in compatibilization of the polymer blend components. The EF‐PLA modified polymer blends have improved melt strength and the resultant films showed better processability as seen by increased bubbled stability. This allowed for blown films with higher PLA content (70%) compared to the unmodified control films (40%). The static charge build‐up typically experienced with PLA film blowing was decreased with the inclusion of EF‐PLA yielding films with better slip and softness. The compatibilization effect of the EF‐PLA modifiers resulted in significant improvement in mechanical properties. For example, dart test performance was up to four times higher than the control, especially at higher PLA concentrations. Therefore, the rheological enhancement and compatibilization effects of the EF‐PLA reactive modifiers make them ideally suited to create high PLA content films. © 2015 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2016 , 133, 43310.     

Influence of Graphene Oxide on Thermally Induced Shape Memory Behavior of PLA/TPU Blends: Correlation with Morphology,Creep Behavior,Crystallinity, and Dynamic Mechanical Properties

In this study, shape memory is thermally induced in a series of graphene oxide (GO) filled poly(lactic acid)/thermoplastic polyurethane (PLA/TPU) blends, prepared via melt mixing process, and their shape recovery and shape fixity are measured, and the results are correlated with morphology, dynamic mechanical properties, crystallinity and creep recovery behavior. Morphological analysis by scanning and transmission electron microscopy reveals that the blends are immiscible, and GO platelets are mainly localized in the TPU phase of the blends, which lead to smaller and more elongated TPU droplets with improved interfacial adhesion being responsible for the improved shape recovery performance compared to the unfilled blend. A systematic enhancement found in storage and Young's modulus, tensile strength, creep resistance and creep recovery, and cold crystallinity as a result of GO inclusion are in agreement with the improved shape recovery, shape fixity and overall shape memory performance of the filled systems. The developed PLA/TPU/GO nanocomposites with highly improved mechanical properties can be utilized as a new class of environmentally friendly shape memory materials for a broad range of applications.     

Poly(lactic acid)–thermoplastic poly(ether)urethane composites synergistically reinforced and toughened with short carbon fibers for three‐dimensional printing

In this study, we prepared short‐carbon‐fiber (CF)‐reinforced poly(lactic acid) (PLA)–thermoplastic polyurethane (TPU) blends by melt blending. The effects of the initial fiber length and content on the morphologies and thermal, rheological, and mechanical properties of the composites were systematically investigated. We found that the mechanical properties of the composites were almost unaffected by the fiber initial length. However, with increasing fiber content, the stiffness and toughness values of the blends were both enhanced because of the formation of a TPU‐mediated CF network. With the incorporation of 20 wt % CFs into the PLA–TPU blends, the tensile strength was increased by 70.7%, the flexural modulus was increased by 184%, and the impact strength was increased by 50.4%. Compared with that of the neat PLA, the impact strength of the CF‐reinforced composites increased up to 1.92 times. For the performance in three‐dimensional printing, excellent mechanical properties and a good‐quality appearance were simultaneously obtained when we printed the composites with a thin layer thickness. Our results provide insight into the relationship among the CFs, phase structure, and performance, as we achieved a good stiffness–toughness balance in the PLA–TPU–CF ternary composites. © 2018 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2018 , 135, 46483.     

Electrospun PLA/PCL fibers with tubular nanoclay: Morphological and structural analysis

Biodegradable polymers are good candidates for a wide range of applications in tissue engineering and drug delivery because of their biocompatibility, their degradation, mechanical properties, and offer a sustained release of encapsulated drugs. The electrospun polymer nanofibrous materials can be used as carriers for hydrophobic and hydrophilic drugs. This research work focused on poly(lactic acid) (PLA) and blends of PLA with poly (ε‐caprolactone) (PCL) that are reinforced with different concentrations of halloysite nanotubes (HNTs) and various cosolvents for electrospinning including chloroform : acetone, chloroform : methanol, and dichloromethane (DCM) : N,N, dimethylformamide (DFM). The fibers produced from the DCM : DMF system without HNTs were more uniform resulting in smaller fiber diameters as compared to the chloroform: methanol system due to the increased solution conductivity. The addition of HNT nanoparticles produced electrospun fibers with large diameters because the viscosity of the solution increased. Cosolvent was important in determining fiber diameters because it strongly influenced the solution viscosity and conductivity. HNTs had relatively small impact on the growth of a crystalline morphology in PCL–HNT composites. The solvent mixture of chloroform : methanol was better for PLA‐based systems since PLA was found to have slightly higher crystallinity and larger enthalpy value indicating the improved structural orderness in the PLA polymer matrix. © 2011 Wiley Periodicals, Inc. J Appl Polym Sci, 2012     

Study of morphology influence on rheological properties of compatibilized TPU/SAN blends

The compatibilizing efficiency of three different compatibilizers on the thermoplastic polyurethane/styrene‐co‐acrylonitrile (TPU/SAN) blends properties was investigated after compatibilizer's incorporation via melt‐mixing. The compatibilizers studied were as follows: poly‐ε‐caprolactone (PCL) of different molecular weight (M_w), a mixture of polystyrene‐block‐polycaprolactone (PS‐b‐PCL) and polystyrene‐block‐poly (methyl methacrylate) (PS‐b‐PMMA), and a mixture of polyisoprene‐block‐polycaprolactone (PI‐b‐PCL) and polybutadiene‐block‐poly (methyl methacrylate) (PB‐b‐PMMA). In our study, the effect of 5 wt % added compatibilizers on TPU/SAN blends morphology was examined. The transmission electron microscopy (TEM) was used to study the morphology at different length scales and to determine the compatibilizer's location. Investigations showed the different improvement of properties, because of the different incorporation of compatibilizers in the polymer blend. The morphology influence on the rheological behavior of compatibilized blends was investigated with a stress‐controlled rheometer (Rheometric Dynamic Stress Rheometer, SR‐500). Different compatibilization activity was found for different system. It was also found that compatibilization activity of added compatibilizer strongly depends on the comaptibilizer's M_w. Blends compatibilized with PCL showed superior properties as compared with the other examined blends. © 2006 Wiley Periodicals, Inc. J Appl Polym Sci 100: 2303–2316, 2006     

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     

Annealing effect on the shape memory properties of polylactic acid (PLA)/thermoplastic polyurethane (TPU) bio-based blends

PLA and TPU were melt-blended to form shape memory bio-based blends with or without post-annealing effect. To the authors’ best knowledge, this is the first work to discuss the annealing effect on the PLA-based SMP blends. Annealed TPU showed regularly fractured surfaces unlike the macro-phase segregated domains for non-annealed TPU. After 3 h-annealing treatment, spherulites were observed for PLA, but not for TPU. The crystallinity of PLA increased, close to 3-fold increment, for annealed blends in comparison with non-annealed blends. The shape memory behaviors of PLA/TPU blends predeformed under three different predeformation temperatures (25, 80, 120 °C) were investigated. The annealing effect was helpful in enhancing the shape fixing ratio of the PLA/TPU (60/40) blend at high predeformation temperature of 120 °C in comparison with 25 °C. However, the suitable selection of the optimum predeformation temperature at 80 °C outweighed the annealing effect to attain the high shape fixing ratio, even in the case of non-annealed blends. The annealing effect often increased the perfection of crystal domains/interfaces and the larger crystal sizes, which would be detrimental to the molecular extensibility. The overall annealing effect on the shape recovery ratios were quite effective for both PLA/TPU blends of 80/20 and 60/40 without sacrificing the shape fixing ratios at the optimum predeformation temperature of 80 °C, attributing to the increased crystallinity of PLA and homogenized phase domains of TPU. Particularly, the annealing treatment did significantly increase the recovery ratio of the blends, more than 2-fold increment, especially for PLA/TPU (60/40) blend. At both lower or higher predeformation temperatures, the stress concentration between the increased crystalline domains and amorphous regions tended to dominate the annealing effect, leading to a negative contribution to the shape recovery processes.