Glassy Region Research Articles

Molecular Ball Joints: Mechanochemical Perturbation of Bullvalene Hardy-Cope Rearrangements in Polymer Networks.

The solution-state fluxional behavior of bullvalene has fascinated physical organic and supramolecular chemists alike. Little effort, however, has been put into investigating bullvalene applications in bulk, partially due to difficulties in characterizing such dynamic systems. To address this knowledge gap, we herein probe whether bullvalene Hardy-Cope rearrangements can be mechanically perturbed in bulk polymer networks. We use dynamic mechanical analysis to demonstrate that the activation barrier to the glass transition process is significantly elevated for bullvalene-containing materials relative to "static" control networks. Furthermore, bullvalene rearrangements can be mechanically perturbed at low temperatures in the glassy region; such behavior facilitates energy dissipation (i.e., increased hysteresis energy) and polymer chain alignment to stiffen the material (i.e., increased Young's modulus) under load. Computational simulations corroborate our work that showcases bullvalene as a reversible "low-force" covalent mechanophore in the modulation of viscoelastic behavior.

Thermo‐mechanical properties of epoxy composites filled with inorganic particulate fillers for robust solder mask application

AbstractFiller components play a crucial role as thermo‐mechanical reinforcement to the epoxy‐based solder mask, ensuring effective insulation and passivation. This study investigates the impact of different inorganic filler types (talc, silica (SiO2), boron nitride (BN) and barium sulfate (BaSO4)) and loadings (5 and 15 wt%) on the tensile and thermal properties of the epoxy composites. The composites were blended, cast and thermally cured. Of these composites, only 15 wt% SiO2/epoxy composite exhibits notable increments in both tensile strength and modulus, surpassing unfilled epoxy by 11.65% and 31.9%, respectively. It also displays the highest elongation at break, supported by small particle size, high specific surface area and minimal void volume fraction. For thermal tests, the addition of all fillers increases the storage modulus in both glassy and rubbery regions, especially 15 wt% talc/epoxy composite with 30.09% increment at 25 °C. Additionally, all fillers raise the glass transition temperature (Tg), notably improving it by 9 °C in the 15 wt% BN/epoxy composite. Moreover, their inclusion generally enhances the onset decomposition temperature (Tonset) and reduces weight loss during decomposition. © 2024 Society of Chemical Industry.

Rationally designed phosphate-doped zinc-cobalt based MOFs wrapped ZnAl-LDH decorated LGO; towards designing epoxy coating with enhanced mechanical & thermal properties

Epoxy coatings application in industries has been broadened due to their exceptional features. However, the high brittleness and poor fracture resistance are two major drawbacks of the epoxy coating (EPC) that limit its durability in harsh outdoor conditions. Advanced nanomaterials i.e., GO have been noticed in recent studies as powerful candidates for resolving epoxy weaknesses. However, the improper dispersion, as well as the weak interaction of GO with epoxy, are the most important challenging issues that remain unsolved. For the first time, GO was reduced and then assembled with the LDH and metal–organic frameworks (i.e., ZF-8, ZF-67) to reach high dispersion levels and strong interactions with the polymer matrix for improving the coating thermal/mechanical characteristics simultaneously.TGA test outcomes declared about 2947% and 2895% increment levels in the EPC thermal resistance after the inclusion of the phosphate-doped LGO@LDH-ZF-67/ZF-8 and LGO@LDH-ZF-8/ZF-67 nanostructures. Tensile test results revealed that in the presence of the phosphate-doped LGO@LDH-ZF-67/ZF-8 and LGO@LDH-ZF-8/ZF-67 nanostructures about 178% and 163%, respectively, improvements in the fracture energy (FE) of the EPC were achieved. According to the DMTA test outcomes, the phosphate-doped LGO@LDH-ZF-67/ZF-8 containing EPC showed 191% and 16% improvements in storage modulus at the glassy region and cross-linking density, respectively.

All-atom molecular dynamics simulation of solvent diffusion in an unentangled polystyrene film.

The diffusion behavior of low molecular weight solvents within an unentangled polystyrene film below and above its glass transition temperature is investigated. The diffusion behavior in the glassy state exhibits a distinct behavior known as case II or class II diffusion, noticeably diverging from conventional Fickian diffusion observed above the glass transition temperature of the polymer film. In the context of case II diffusion, the primary experimental observation entails the emergence of a well-defined concentration front moving at a constant speed, delineating a swollen, rubbery region from a glassy region within the polymer system. Despite the prevalence of this phenomenon in experimental settings, simulating case II diffusion has posed a significant challenge, primarily due to the computationally intensive nature of the diffusion process. To address this, we have developed an all-atom molecular dynamics simulation approach for the observation of case II diffusion in glassy polymers. This method aims to unravel the intricacies of the diffusion process, providing valuable insights into the dynamic interactions between solvents and the polymer matrix.

A novel simulation model to analyze rice intermittent drying considering glass transition concept

During rice drying its starch exhibits a variety of thermal properties. It can be transformed from a rubbery state to a glassy state and vice versa due to temperature and moisture content gradients (MCGs) leading to the reduction in head rice yield. Intermittent drying is an effective drying method to overcome this issue. In this research, a novel mathematical model was developed for rice intermittent drying process considering the glass transition concept which has not been done before. In addition, the real 3D body-fitted geometry of the rice kernel was first utilized for simulation. To determine the required coefficients and validate the model, continuous and two-stage intermittent drying (2SID) experiments were performed. A correlation of 99% was found between the drying kinetics obtained from the experiments and those obtained from the model. Regarding the glass transition phenomenon, a quantitative S function was defined to express the local glassy-to-rubbery state at each time. The transitory temperature and moisture distributions inside the rice kernel were displayed and discussed at each stage of the 2SID. Further, the glass transition behavior of the rice kernels was investigated by using the S function's values. The glassy region extended by 28.8%, 3.3%, and 20.1% of the whole kernel rice at the first drying, tempering, and second drying stages, respectively. At the end of the 2SID, 45.6% of the entire kernel was located in the glassy region while the central layers were still located in the rubbery region. Overall, the developed model could be used to determine the optimal intermittent drying parameters for rice to improve its dehydration performance at a low cost.

Influence of fly ash on thermo-mechanical and mechanical behavior of injection molded polypropylene matrix composites

Polypropylene composites find widespread application in industries, including packaging, plastic parts, automotive, textiles, and specialized devices like living hinges known for their remarkable flexibility. This study focuses on the manufacturing of polypropylene composite specimens by incorporating varying weight percentages of fly ash particles with polypropylene using a twin-screw extruder and injection molding machine. The composites were comprehensively tested, evaluating tensile, compressive, and flexural strength, solid-state and polymer melt properties, modulus, damping, and thermal response. The findings reveal that the compressive strength of polypropylene increases up to 2 wt% of added fly ash particles and subsequently exhibits a slight decline. Tensile strength demonstrates an increase up to 1 wt% of fly ash, followed by a decrease with a 2 wt% addition, and then a subsequent increase. Flexural strength shows improvement up to 3 wt% fly ash addition before declining. The storage modulus curve is categorized into three regions: the glassy region (up to 0 °C), the glass transition region (0–50 °C), and the glass transition region of polypropylene (>50 °C), each corresponding to different molecular motions. Weight loss curves exhibit similar trends, indicating uniform pyrolysis behavior attributed to consistent chemical bonds. Plastic degradation commences around 440 °C and concludes near 550 °C. Additionally, elemental mapping of fly ash composition identified various elements such as O, Si, K, Mg, Ca, Cl, Na, P, Al, Fe, S, Cu, Ti, and Ni. These findings offer valuable insights into the mechanical and thermal properties of polypropylene composites reinforced with fly ash, rendering them suitable for a wide range of industrial applications necessitating strength and durability across temperature variations.

Dynamic mechanical analysis for assessment of carbon fillers in glass fiber epoxy composites

AbstractThe effect of incorporation of micron sized aluminum trihydrate, multi‐walled carbon nanotubes, and graphene nano platelets into glass fiber reinforced epoxy matrix is investigated using dynamic mechanical analysis. The objective of the investigation was to develop polymer central core of high temperature low sag transmission conductor. The effect of individual and hybrid carbon fillers on the viscoelastic properties of the epoxy composites is investigated and discussed. The storage modulus of the glass reinforced epoxy increases by 20% at room temperature due to incorporation of carbon nanofillers. In glass transition region, the increase is higher between 40% and 60% and it varies up to 90% in the rubbery region. Key attributes of carbon filler addition are limited enhancement of storage modulus at room temperature, higher enhancement over glassy, glass transition, and rubbery regions. The carbon fillers extend the temperature range of the glassy region. The cross‐link density, filler efficiency, and degree of entanglement of fibers are estimated to understand the implications of the carbon fillers on the viscoelastic properties. The loss modulus peak of glass epoxy composite increases from 2800 to 3900 MPa with carbon fillers and the increase in glass transition temperature is 47°C. Incorporation of carbon fillers leads to increase of damping factor peak from 0.2 to 0.28. Cole–Cole plots have established the inherent heterogeneity of epoxy systems due to the presence of carbon fillers. Prediction models for storage modulus and damping factor have been proposed to highlight the influence of geometry and size of carbon filler.

Plasticization, Antiplasticization, and Fragility in Blends of Polyvinyl Butyral and Polyethylene Glycol Dimethyl Ether

AbstractBlends of polyvinyl butyral (PVB) and polyethylene glycol dimethyl ether (PEGDME) with low molecular weight (= 250 g mol−1) show two calorimetric (for PEGDME content higher than 11% by weight) and mechanical glass transitions. Their substantial changes in the relative content of the two components are explained by considering the self‐concentrations of both polymers determined by the connectivity of their own chains. Increasing content of PEGDME lower the glass transition temperature Tg of PVB (the component with the highest Tg) by about 100 K, also causing a progressive and significant increase of its fragility (following the Angell's strong/fragile liquids classification scheme). Strengthening of polymer blends is observed in the fully glassy region, quite below the Tg's of both the components, with the storage modulus E′ becoming more than a factor 2 higher than that of neat PVB. The progressive increase of E′, without any change of slope, points to structural homogeneity of blends determined by compatibility of components, as a result of interchain interactions activated by the polar groups of both polymers. The present results reveal that PEGDME plasticizes PVB when the blend is in the fully rubbery state while acting as an anti‐plasticizer in the fully glassy state.

Microstructure design of porous viscoelastic composites with prescribed relaxation moduli by multi-material topology optimization

This paper presents a multi-material topology optimization method for designing the microstructures of porous viscoelastic composites with prescribed relaxation moduli. It is assumed that the composite materials are microscopically composed of periodic unit cells. The effective relaxation moduli of the composites are obtained using the homogenization method. The density-based topology optimization is utilized, and a related material interpolation scheme is introduced. The design objective is to determine an optimal material distribution that exhibits the prescribed modulus in both the glassy and rubbery regions. The design sensitivity is derived analytically using the adjoint variable method. A filtering scheme is adopted to impose a minimum length scale for each material phase. Several numerical examples are presented to demonstrate the effectiveness of the proposed method. Various microstructures with prescribed relaxation moduli are presented and discussed. In addition, the bounds on the relaxation moduli of the optimized microstructures are compared with theoretical bounds.

Tracking of Formed Crystalline Phases in the Binary Silver Tellurite Glass-ceramics

Glasses and glass-ceramics based on silver tellurite system xAg2O·(100-x)TeO2 (0 £ x £ 60 mol%) were prepared by melt-quenching method. The structure of the studied glasses and glass-ceramics was investigated by several techniques. XRD patterns reveal the existence of only one glassy region at 20 < x ≤ 30 mol% with two crystalline a-TeO2 and Ag2TeO3 phases that formed separately in the prepared samples below 20 and beyond 30 mol% Ag2O, respectively. The peaks intensity corresponding to the crystalline a-TeO2 and Ag2TeO3 phases was found to decrease and increase with Ag2O content, respectively. This may be correlated with changes in the concentration of and units that, respectively, build up the crystalline a-TeO2 and Ag2TeO3 phases. In the glassy region, there is no crystalline phase, which may be attributed to the abundance of the deformed units that build up the glassy phase, and the concentrations of and units are neglected in this region. SEM and TEM micrographs and the related electron diffraction patterns (EDP) confirmed the formation of crystallized clusters in Ag2O-rich glasses.

Thermomechanical and Dielectric Properties Relationship of Hybrid Carbon Black and Nano Silica Epoxy Composites

Multifunctional materials refer to the types of materials that possess enhanced mechanical, electrical, and thermal properties. In this work, nano silica and Carbon Black (CB) are added to epoxy polymer as an effort to improve the thermomechanical and dielectric properties of the composites. Filler loadings are varied from 0.1 wt.%, up till 5 wt.%. The thermomechanical properties are measured from Dynamic Mechanical Thermal Analysis (DMTA) while the dielectric properties are measured from Vector Network Analyser (VNA). The synergistic effects of combining both fillers (keeping them at 1:1 wt.% ratio) are also assessed. It was found that the value of glass transition temperature (Tg) increased from 56.85°C (neat epoxy) to 59.8°C (5 wt.% CB). The Tq values further increased to 64.7°C, for 5 wt.% hybrid fillers (2.5 wt.% silica + 2.5 wt.% CB), demonstrating the synergistic effects by employing dual fillers. By adding single and dual fillers, the values of storage Modulus, E’ remains almost constant for both glassy (40°C) and rubbery region (100°C), regardless of the loadings employed. The values of real permittivity, er’ was also measured for dual fillers in the frequency range between 300 kHz to 18 GHz. The highest value of er’ was 5.5 F/m, which was measured for both 1.5 mm and 2.0 mm sample thickness of 5 wt.% hybrid fillers (2.5 wt.% silica + 2.5 wt.% CB). This study highlights the thermomechanical and dielectric properties improvement of epoxy composites by incorporating dual fillers.

Emergent Glassy Behavior in a Kagome Rydberg Atom Array.

We present large-scale quantum MonteCarlo simulation results on a realistic Hamiltonian of kagome-lattice Rydberg atom arrays. Although the system has no intrinsic disorder, intriguingly, our analyses of static and dynamic properties on large system sizes reveal emergent glassy behavior in a region of parameter space located between two valence bond solid phases. The extent of this glassy region is demarcated using the Edwards-Anderson order parameter, and its phase transitions to the two proximate valence bond solids-as well as the crossover towards a trivial paramagnetic phase-are identified. We demonstrate the intrinsically slow (imaginary) time dynamics deep inside the glassy phase and discuss experimental considerations for detecting such a quantum disordered phase with numerous nearly degenerate local minima. Our proposal paves a new route to the study of real-time glassy phenomena and highlights the potential for quantum simulation of a distinct phase of quantum matter beyond solids and liquids in current-generation Rydberg platforms.

Synthesis and Characterization of Bamboo Employed Environmentally Friendly Cellulose Nanofibrils Reinforced Natural Rubber Composites with Uncompromised Mechanical Properties

In this study, high-purity cellulose nanofibrils (CNFs) were environmentally friendly extracted from natural bamboo. Physical, chemical, and mechanical treatments were comprehensively investigated, and then ensembled to effectively and efficiently remove lignin and hemicellulose with low energy from raw bamboo fibers, which combine microwave liquefaction, hydrogen peroxide-acetic acid delignification, alkaline treatment, and along with acid hydrolysis. This was able to allow for the extraction of CNFs. Compositional analysis, Fourier-transform infrared spectroscopy, X-ray diffraction, X-ray photoelectron spectroscopy, and thermogravimetric analysis were performed to investigate and confirm the successful removal of undesirable lignin and hemicellulose. The resultant cellulose fibers were then subjected to a mechanical treatment to obtain the cellulose nanofibrils. It was found that the obtained CNFs have an average diameter of 13 nm with a cellulose purity of 94.52%. Without any further surface modification, the incorporation of bamboo-based CNFs into natural rubber (NR) exhibits significant improvement in their mechanical properties including modulus (~66.67%), tensile strength (~120.83%), toughness (~139.34%), and elongation at break (~31.41%). Interestingly, there is no compromise between tensile strength and elongation at break for the nanocomposites. DMA results also showed that both storage and loss moduli were dramatically enhanced over those of neat NR in their glassy region, which is typically unusual. This study can show, if optimized for material extraction, the great promise to the potential use of natural materials to develop environmentally friendly composites with multi-functionality in a variety of real-world engineering structural applications.

Determining the Thermal Conductivity of Gehlenite by Thermal Microscopy at Room Temperature

The thermal conductivity of a single-phase gehlenite (2CaO Al2O3 SiO2) sample was determined using thermal microscopy. The composition of the primary crystal region of the gehlenite sample was CaO: SiO2:Al2O3 = 38:28:34 (mass%), which was maintained after melting and cooling. After polishing the samples, the size of the gehlenite crystal was sufficiently large to be measured using a thermal microscope. The value of sqrt{lambda Crho }, where λ is thermal conductivity C is specific heat andρis density, of the samples was measured every 10 μm to obtain its distribution. When comparing the results with the optical microscopy image of the sample, the gehlenite region showed a larger value of sqrt{lambda Crho } than the glassy region. Specifically, the value of sqrt{lambda Crho } of the gehlenite region was determined to be 2.2 ± 0.1 kJs−0.5·m−2·K−1, which resulted in a thermal conductivity of 2.1 ± 0.2 Wm−1·K−1. Moreover, the oxide gehlenite phase showed lower thermal conductivity than the other constituent phases, i.e., CaO, Al2O3, and SiO2.

Dynamic viscoelastic behavior and interlaminar performance of glass/epoxy composites with binary nano‐fillers at different in‐situ elevated temperature environments

AbstractFor commercial civil applications of laminated composite material, characterizations to forecast the interlaminar shear behavior and viscoelastic response across a wide temperature range are essential. In this study, the interlaminar shear strength (ILSS) of glass/epoxy (GE) composites dispersed with binary nanofillers nanosilica‐multilayer graphene (NS‐MLG) and nanosilica‐nanoclay (NS‐NC) was analyzed at an in‐situ testing temperature of 20, 70, and 110°C. Further, the viscoelastic property of the composites was studied using a dynamic mechanical thermal analyzer (DMTA) in the temperature range of 35–165°C. An increase in the ILSS value of around 9% and 10% was observed at room temperature for GE/MLG‐NS and GE/NC‐NS, respectively, compared to control GE composites. In contrast, the trend was seen to change at higher temperatures. There was a slight decrement in the storage modulus (E′) of GE/MLG‐NS and GE/NC‐NS composites in the glassy region compared to control GE composites. The mean Tg of the GE composite (control) was nearly 107.3°C when the E′ decline onset temperature was taken into account, but after the addition of MLG‐NS, it was 10.1°C below. The mean Tg of GE/NC‐NS was determined to be 106.3°C, and in the glass transition as well as rubbery regions, it was observed to compete with the E′ value of the control GE composites. Fractography was done using micrographs obtained from environmental scanning electron microscope (ESEM). Traces of polymeric material found at the fiber surface certified the improved interfacial adhesion between glass fiber and polymer in the matrix‐modified composite samples.

Sequence-Enhanced Self-Healing in "Lock-and-Key" Copolymers.

Van der Waals-driven self-healing in copolymers with "lock-and-key" architecture has emerged as a concept to endow engineering-type polymers with the capacity to recover from structural damage. Complicating the realization of "lock-and-key"-enabled self-healing is the tendency of copolymers to form nonuniform sequence distributions during polymerization reactions. This limits favorable site interactions and renders the evaluation of van der Waals-driven healing difficult. Here, methods for the synthesis of lock-and-key copolymers with prescribed sequence were used to overcome this limitation and enable the deliberate synthesis of "lock-and-key" architectures most conducive to self-healing. The effect of molecular sequence on the material's recovery behavior was evaluated for the particular case of three poly(n-butyl acrylate/methyl methacrylate) [P(BA/MMA)] copolymers with similar molecular weights, dispersity, and overall composition but with different sequences: alternating (alt), statistical (stat), and gradient (grad). They were synthesized using atom transfer radical polymerization (ATRP). Copolymers with alt and stat sequence displayed a 10-fold increase of recovery rate compared to the grad copolymer variant despite a similar overall glass transition temperature. Investigation with small-angle neutron scattering (SANS) revealed that rapid property recovery is contingent on a uniform microstructure of copolymers in the solid state, thus avoiding the pinning of chains in glassy MMA-rich cluster regions. The results delineate strategies for the deliberate design and synthesis of engineering polymers that combine structural and thermal stability with the ability to recover from structural damage.

Graphene oxide nano-layers functionalized/reduced by L-Citrulline/Pectin bio-molecules for epoxy nanocomposite coating mechanical properties reinforcement

In this work, graphene oxide (GO) was reduced/modified by an eco-friendly route using L-Citrulline molecules extracted from the watermelon rind. Before and after the modification/reduction process, the rGO layers were characterized by different spectroscopy techniques. In addition, the mechanical properties of the epoxy-rGO reinforced coatings were evaluated by tensile and dynamic mechanical thermal analysis (DMTA) tests. The characterization results have demonstrated that the GO nanosheets were successfully reduced/modified by the extracted compounds. DMTA analysis showed that the values of storage modulus at glassy and rubbery regions for the neat epoxy sample incorporated with the rGO nanosheets were increased by about 39 % and 97 %, respectively. Moreover, the glass transition temperature (Tg) was increased from 76.8 °C for the neat epoxy (EP) to 84.0 °C for the EP/modified-reduced GO nanocomposite. Tensile tests showed that the values of tensile strength, maximum strain, elastic modulus, and toughness of the epoxy-based coating were respectively increased by about 142 %, 266 %, 46.7 %, and 388 % after incorporation of the rGO nanosheets compared to the EP sample.

Recycling Waste Nonmetallic Printed Circuit Boards for Polyvinyl Chloride Composites.

To reduce environmental threats, such as land filling, incineration and soil pollution, which are associated with the improper waste management of waste printed circuit boards, the utilization of NMPCBs from waste PCBs as a filler in composites was pursued. Untreated and treated NMPCBs in varying ratios, 10–30 wt.%, were blended with PVC to produce NMPCB/PVC composites, using the melt-mixing method via an internal mixer, in order to solve the remaining NMPCB waste problem after the valuable metals in PCBs were recovered. The incorporation of the NMPCB with PVC resulted in an increase in the tensile modulus and the thermal stability of the resulting composites. Scanning electron microscopy (SEM) results indicated improved interfacial adhesion between the treated NMPCB and the PVC matrix. The FTIR results of the NMPCB treated with 3-glycidyloxypropyltrimethoxysilane (GPTMS) revealed the formation of Si-O-Si bonds. The densities of the composites were found to increase with an increase in the content of the treated NMPCB, and compatibility improved. The tensile properties of the treated NMPCB/PVC composites were higher than those of the untreated NMPCB/PVC composites, suggesting improved compatibility between the treated NMPCB and PVC. The PVC composite with 10 wt.% of the treated NMPCB showed the optimum tensile properties. It was observed that the tensile modulus of the treated NMPCB/PVC composite increased by 47.65% when compared to that of the neat PVC. The maximum thermal degradation temperature was 27 °C higher than that of the neat PVC. Dynamic mechanical analysis results also support the improved interfacial adhesion as a result of the improvement in the storage modulus at the glassy region, and the loss factor (tan δ) peak shifted to a higher temperature range than that of the PVC and the untreated NMPCB/PVC composite. These studies reveal that the NMPCB was successfully modified with 1 wt.% of GPTMS, which promoted the dispersion and interfacial adhesion in the PVC matrix, resulting in better tensile properties and better thermal stability of the PVC composite.

Thermomechanical and optical characteristics of nanoquartz‐ and nanozircon‐filled poly(methyl methacrylate) composites

AbstractThe thermomechanical and optical properties of poly(methyl methacrylate) (PMMA)/quartz and PMMA/zircon composites at filler content variations of 0, 1, 2.5, and 5 wt% have been studied. The silica quartz and zircon powders were derived from local sands collected from Tanah Laut, South Kalimantan, and Kereng Pangi, Central Kalimantan, Indonesia, respectively. The nanoquartz and nanozircon fillers (herewith were designated as quartz and zircon respectively) were obtained by milling these powders for 15 h. Dynamic mechanical analysis was used to acquire the storage modulus and glass transition temperature as the thermomechanical properties of the PMMA/quartz and PMMA/zircon composites. Meanwhile, the optical properties were determine using ultraviolet–visible spectroscopy. Results indicate that zircon fillers can improve the storage modulus of the composites up to 1.85 times that of PMMA alone. Zircon is more effective than silica in improving the storage modulus of PMMA. Implementing the degradation rate model shows us that all the composites have nearly the same degradation behavior in the glassy region. Moreover, the addition of fillers decreases the band gap energies.

Tunable mechanical properties of glass fiber/epoxy composites by incorporating bioinspired montmorillonite–carbon nanotube/epoxy interface layer around the fiber

The mutual exclusiveness between strength and toughness restricts the engineering application of glass fiber/epoxy composites requiring both high strength and suitable toughness. Inspired by natural nacre, a hetero-structural montmorillonite−multiwalled carbon nanotube (Mt−MWCNT) hybrid was coated on the curved surface of glass fibers to construct a nacre-like interface layer, consisting of Mt as “brick”, MWCNTs as “anchor” and initial epoxy resin as “mortar”. MWCNTs were employed for guaranteeing the effective separation of Mt nanosheets and strong interfacial interactions among the Mt, matrix and fiber. The enhanced dispersion degree of Mt−MWCNT hybrids and strongly bonded interface layer were established, and synergistic effects of Mt and MWCNTs on the strength and toughness of composites were also demonstrated. Compared with pure glass fiber/epoxy composite, interlaminar shear strength and work of break of resulting composites were improved by approximately 28% and 189%, respectively; meanwhile, such composite exhibits higher storage modulus in the glassy region and superior thermal stability. This work demonstrates a practical and effective strategy for fabricating high-performance yet low-cost fiber-reinforced composites through the nature-inspired interface.