Nacre-like block lattice metamaterials with targeted phononic band gap and mechanical properties.

The extraordinary quasi-static mechanical properties of nacre-like composite metamaterials, such as high specific strength, stiffness, and toughness, are due to the periodic arrangement of two distinct phases in a "brick and mortar" structure. It is also theorized that the hierarchical periodic structure of nacre structures can provide wider band gaps at different frequency scales. However, the function of hierarchy in the dynamic behavior of metamaterials is largely unknown, and most current investigations are focused on a single objective and specialized applications. Nature, on the other hand, appears to develop systems that represent a trade-off between multiple objectives, such as stiffness, fatigue resistance, and wave attenuation. Given the wide range of design options available to these systems, a multidisciplinary strategy combining diverse objectives may be a useful opportunity provided by bioinspired artificial systems. This paper describes a class of hierarchically-architected block lattice metamaterials with simultaneous wave filtering and enhanced mechanical properties, using deep learning based on artificial neural networks (ANN), to overcome the shortcomings of traditional design methods for forward prediction, parameter design, and topology design of block lattice metamaterial. Our approach uses ANN to efficiently describe the complicated interactions between nacre geometry and its attributes, and then use the Bayesian optimization technique to determine the optimal geometry constants that match the given fitness requirements. We numerically demonstrate that complete band gaps, that is attributed to the coupling effects of local resonances and Bragg scattering, exist. The coupling effects are naturally influenced by the topological arrangements of the continuous structures and the mechanical characteristics of the component phases. We also demonstrate how we can tune the frequency of the complete band gap by modifying the geometrical configurations and volume fraction distribution of the metamaterials. This research contributes to the development of mechanically robust block lattice metamaterials and lenses capable of controlling acoustic and elastic waves in hostile settings.

Preparation of photoluminescent nano-biocomposite nacre from graphene oxide and polylactic acid.

Nano-biocomposites of inorganic and organic components wereprepared to produce long-persistent phosphorescent artificial nacre-like materials. Biodegradable polylactic acid (PLA), graphene oxide (GO), and nanoparticles (13-20 nm) of lanthanide-doped aluminate pigment (NLAP) were used in a simple production procedure of an organic/inorganic hybrid nano-biocomposite. Both polylactic acid and GO nanosheets were chemically modified to form covalent and hydrogen bonding. The high toughness, good tensile strength, and great endurance of those bonds were achieved by their interactions at the interfaces. Long-persistent and reversible photoluminescence was shown by the prepared nacre substrates. Upon excitation at 365 nm, the nacre substrates generated an emission peak at 517 nm. When ultraviolet light was shone on luminescent nacres, they displayed a bright green colour. The high superhydrophobicity of the generated nacres was obtained without altering their mechanical characteristics.

Myriad Mapping of nanoscale minerals reveals calcium carbonate hemihydrate in forming nacre and coral biominerals.

Calcium carbonate (CaCO3) is abundant on Earth, is a major component of marine biominerals and thus of sedimentary and metamorphic rocks and it plays a major role in the global carbon cycle by storing atmospheric CO2 into solid biominerals. Six crystalline polymorphs of CaCO3 are known-3 anhydrous: calcite, aragonite, vaterite, and 3 hydrated: ikaite (CaCO3·6H2O), monohydrocalcite (CaCO3·1H2O, MHC), and calcium carbonate hemihydrate (CaCO3·½H2O, CCHH). CCHH was recently discovered and characterized, but exclusively as a synthetic material, not as a naturally occurring mineral. Here, analyzing 200 million spectra with Myriad Mapping (MM) of nanoscale mineral phases, we find CCHH and MHC, along with amorphous precursors, on freshly deposited coral skeleton and nacre surfaces, but not on sea urchin spines. Thus, biomineralization pathways are more complex and diverse than previously understood, opening new questions on isotopes and climate. Crystalline precursors are more accessible than amorphous ones to other spectroscopies and diffraction, in natural and bio-inspired materials.

Physical Phenomena Governing Mineral Morphogenesis in Molluscan Nacre.

Mollusks, as well as many other living organisms, have the ability to shape mineral crystals into unconventional morphologies and to assemble them into complex functional mineral-organic structures, an observation that inspired tremendous research efforts in scientific and technological domains. Despite these, a biochemical toolkit that accounts for the formation of the vast variety of the observed mineral morphologies cannot be identified yet. Herein, phase-field modeling of molluscan nacre formation, an intensively studied biomineralization process, is used to identify key physical parameters that govern mineral morphogenesis. Manipulating such parameters, various nacre properties ranging from the morphology of a single mineral building block to that of the entire nacreous assembly are reproduced. The results support the hypothesis that the control over mineral morphogenesis in mineralized tissues happens via regulating the physico-chemical environment, in which biomineralization occurs: the organic content manipulates the geometric and thermodynamic boundary conditions, which in turn, determine the process of growth and the form of the biomineral phase. The approach developed here has the potential of providing explicit guidelines for the morphogenetic control of synthetically formed composite materials.

Nacre-inspired composite paper of PVA crosslinked basalt scale and nanocellulose with enhanced mechanical, electrical insulating and ultraviolet-resistant aging performance.

Silicate scales are commonly incorporated into cellulose nanofiber (CNF) as functional fillers to enhance electrical insulation and UV-shielding properties. Nevertheless, the addition of substantial quantities of silicate scales in the quest for enhanced functional properties results in reduced interface bonding capability and compromised mechanical properties, thereby restricting their application. Here, inspired from nacre, layered composite paper with excellent mechanical strength, electrical insulation and UV-resistance properties was fabricated through vacuum assisted self-assembly using CNF, PVA and basalt scales (BS). Unlike the conventional blending strategy, the pre-mixed PVA and BS suspension facilitates the formation of Al-O-C bond, thereby enhancing the interfacial bonding between BS and CNF. Consequently, the composite paper (BS@PVA/PVA/CNF) containing 60 wt% BS demonstrates higher mechanical strength-approximately 140 % higher than that of BS/CNF composite paper, achieving a strength of 33.5 MPa. Additionally, it demonstrates enhanced dielectric properties, surpassing those of CNF paper by up to 107 %. Moreover, it exhibits robust ultraviolet-resistant aging performance, retaining ~87 % of its tensile strength after undergoing a simulated two-year aging period. As a result, this work presents a simple and innovative design strategy for enhancing interfacial bonding and optimizing layer structure, providing essential guidelines for large-scale production of high-performance insulation and aging-resistant composite paper.

Enhancing stiffness and damping characteristics in nacreous composites through functionally graded tablet design.

Nacreous composites offer significant potential for applications in structural damping materials, which require simultaneous high stiffness and damping properties. In this study, we propose that the incorporation of functionally graded tablets into nacreous composites can further enhance both stiffness and damping energy dissipation concurrently. Analytical formulae for the loss modulus, storage modulus, and loss factor, validated through a series of finite element analyses, were derived to investigate the effects of variations in tablet modulus, structural geometry, and constituent properties. Our analyses demonstrate that designing a parabolic modulus distribution in the tablets can yield optimal strengthening and damping results. Furthermore, the characteristic modulus variation degree, overlap length, and frequency emerged from the systematic optimization of loss and storage moduli. Additionally, numerical experiments and model predictions demonstrate that the loss modulus of functionally graded nacreous composites surpasses the predetermined design limit and is five times greater than that of existing homogeneous nacreous composites. Combining the developed theoretical model presented here with advanced 3D printing techniques would offer effective guidelines for designing and fabricating high-performance bio-inspired structural damping composites.

Nacre-like ceramic composites: Properties, functions and fabrication in the context of dental restorations.

Dental restorations are in increasing demand, yet their success rate strongly decreases after 5-10 years post-implantation, attributed in part to mismatching properties with the surrounding buccal environment that causes failures and wear. Among current research to address this issue, biomimetic approaches are promising. Nacre-like ceramic composites are particularly interesting because they combine multiple antagonistic properties making them more resistant to failure in harsh environment than other materials. With the rapid progress in 3D printing producing nacre-like structures has open up new opportunities not yet realised. In this paper, nacre-like composites of various compositions are reviewed in the context of hypothetical biomimetic dental restorations. Their structural, functional and biological properties are compared with those of dentin, enamel, and bone to determine which composition would be the most suitable for each of the 3 mineralized regions found in teeth. The role of complex microstructures and mineral orientations are discussed as well as 3D printing methods that allow the design and fabrication of such complex architectures. Finally, usage of these processes and anticipated prospects for next generation biomimetic dental replacements are discussed to suggest future research directions in this area. STATEMENT OF SIGNIFICANCE: With the current ageing population, dental health is a major issue and current dental restorations still have shortcomings. For the next generation of dental restorations, more biomimetic approaches would be desirable to increase their durability. Among current materials, nacre-like ceramic composites are interesting because they can approach the various structural properties found in the different parts of our teeth. Furthermore, it is also possible to embed self-sensing functionalities to enable monitoring of oral health. Finally, new recent 3D printing technologies now permit the fabrication of complex shapes with local compositions and local microstructures. With this current status of the research, we anticipate new dental restorations designs and highlight the remaining gaps and issues to address.

Bio-inspired nacre-like zirconia/PMMA composites for chairside CAD/CAM dental restorations.

OBJECTIVES: To introduce a versatile fabrication process to fabricate zirconia/PMMA composites for chairside CAD/CAM dental restorations. These zirconia composites have nacre-like lamellar microstructures, competent and tooth-matched mechanical properties, as well as crack resistance behaviours. METHODS: Bi-directional freeze casting was used to fabricate ceramic green bodies with highly aligned lamellar structure. Pressure was then applied to control the ceramic volume fraction. PMMA was infiltrated into the ceramic scaffold. Mechanical tests including 3-point bending, Vickers hardness, and fracture toughness were performed on the composites. The machinability of the composites was also characterised. RESULTS: Two types of nacre-like zirconia/PMMA composites, i.e., 3Y-YZP/PMMA and 5Y-PSZ/PMMA composites were fabricated. The microstructure created was similar to the 'brick and mortar' structure of nacre. Excellent flexural strength (up to 400 MPa and 290 MPa for 3Y-TZP/PMMA and 5Y-PSZ/PMMA composite, respectively), tuneable hardness and elastic modulus within the range similar to enamel, along with improved crack-resistance behaviour were demonstrated on both zirconia composites. In addition, both zirconia/PMMA composites showed acceptable machinability, being easy to mill, as would be required to produce a dental crown. SIGNIFICANCE: Nacre-like zirconia/PMMA composites therefore exhibit the potential for use in the production of chairside CAD/CAM dental restorations.

Transcriptome and exosome proteome analyses provide insights into the mantle exosome involved in nacre color formation of pearl oyster Pinctada fucata martensii.

Color polymorphisms in molluscan shells play an important economic in the aquaculture industry. Among bivalves, shell color diversity can reflect properties such as growth rate and tolerance. In pearl oysters, the nacre color of the donor is closely related to the pearl color. Numerous genes and proteins involved in nacre color formation have been identified within the exosomes of the mantle. In this study, we analyzed the carotenoids present in the mantle of gold- and silver-lipped pearl oysters, identifying capsanthin and xanthophyll as crucial pigments contributing to coloration. Transcriptome analysis of the mantle revealed several differentially expressed genes (DEGs) involved in color formation, including ferric-chelate reductase, mantle genes, and larval shell matrix proteins. We also isolated and identified exosomes from the mantles of both gold- and silver-lipped strains of the pearl oyster Pinctada fucata martensii, revealing the extracellular transition mechanism of coloration-related proteins. From these exosomes, we obtained a total of 1223 proteins, with 126 differentially expressed proteins (DEPs) identified. These proteins include those associated with carotenoid metabolism and Fe(III) metabolism, such as apolipoproteins, scavenger receptor proteins, ß,ß-carotene-15,15'-dioxygenase, ferritin, and ferritin heavy chains. This study may provide a new perspective on the nacre color formation process and the pathways involved in deposition within the pearl oyster P. f. martensii.

Dietary supplementation with nacre reduces cortical bone loss in aged female mice.

Aging is associated with detrimental bone loss leading to fragility fractures in both men and women. Notably, a majority of bone loss with aging is cortical, as well as a large number of fractures are non-vertebral and at the non-hip sites. Nacre is a product of mollusks composed of calcium carbonate embedded in organic components. As our previous study demonstrated the protective effect of nacre supplementation on trabecular bone loss in ovariectomized rats, we sought to evaluate the effect of dietary nacre on bone loss related to aging in female mice which do not suffer true menopause as observed in women. The current study compared the effect of a 90-day long nacre-supplemented diet to that of Standard or CaCO3 diets on both bone mass and strength in 16-month-old C57BL/6 female mice. Multiple approaches were performed to assess the microarchitecture and mechanical properties of long bones, analyze trabecular histomorphometry, and measure bone cell-related gene expressions, and bone turnover markers. In the cortex, dietary nacre improved cortical bone strength in line with lower expression levels of genes reflecting osteoclasts activity compared to Standard or CaCO3 diets (p < 0.05). In the trabeculae, nacre-fed mice were characterized by a bone remodeling process more active than the other groups as shown by greater histomorphometric parameters and osteoblast-related gene expressions (p < 0.05). But these differences were not exhibited at the level of the trabecular microarchitecture at this age. Collectively, these data suggest that dietary nacre should be a potential candidate for reducing aging-associated cortical bone loss in the elderly.

Nacre-Inspired MXene Nanocomposite-based Strain Sensor with Ultrahigh Sensitivity in a Small Strain Range for Parkinson's Disease Diagnosis.

Nowadays, chronic diseases are the primary threat to public health and are getting younger. By taking the advantages of continuousness, convenience, and real-time response, wearable strain sensors have been given great attention to diagnose chronic diseases via analyzing the patient's health state. However, most physiological signals, such as limb tremor of Parkinson's disease, microexpression, and slight joint movement, are tiny and difficult to be detected. Therefore, the development of strain sensors characterized with ultrahigh sensitivity in a small strain range (ε < 10%) is urgent. Inspired by nacre's hierarchical structure, we have fabricated nacre-mimetic nanocomposites with "brick-and-mortar" architecture by employing polyacrylamide (PAM) and Ti3C2Tx MXene nanosheets through a layer-by-layer (LBL) spin-coating technique. The resultant nanocomposite-based strain sensor exhibits ultrahigh sensitivity in a small strain range (GF = 296.8, ε < 10%), attributed to the bioinspired hierarchical structure and hydrogen bond-enhanced interfacial interactions. In addition, a high reliability, broad working sensing range (453%), short response time (183 ms), skin-like tensile stress (7.2 MPa), and excellent durability (2000 cycles) are also achieved. Due to the ultrahigh sensitivity within a small strain, the reported strain sensor can accurately diagnose and distinguish Parkinson's disease symptoms, including thumb pill-rolling tremor, masked face (microexpression), intermittent shaking of the head, and limb cogwheel motion. This work provides new insights to design strain sensors with high sensitivity for monitoring tiny signals and for disease diagnosis.

Impact of ocean acidification on shells of the abalone species Haliotis diversicolor and Haliotis discus hannai.

Ocean acidification (OA) results from the absorption of anthropogenic CO2 emissions by the ocean and threatens the survival of many marine calcareous organisms including molluscs. We studied OA effects on adult shells of the abalone species Haliotis diversicolor and Haliotis discus hannai that were exposed to three pCO2 conditions (ambient, ∼880, and ∼1600 µatm) for 1 year. Shell periostracum corrosion under OA was observed for both species. OA reduced shell hardness and altered the nacre ultrastructure in H. diversicolor, making its shells more vulnerable to crushing force. OA exposure did not reduce the shell hardness of H. discus hannai and did not alter nacre ultrastructure. However, the reduced calcification also decreased its resistance to crushing force. Sr/Ca in the shell increased with rising calcification rate. Mg/Ca increased upon OA exposure could be due to a complimentary mechanism of preventing shell hardness further reduced. The Na/Ca distribution between the aragonite and calcite of abalone shells was also changed by OA. In general, both abalone species are at a greater risk in a more acidified ocean. Their shells may not provide sufficient protection from predators or to transportation stress in aquaculture.

Nacre-inspired, strong, tough silk fibroin hydrogels based on biomineralization and the layer-by-layer assembly of ordered silk fabric.

Hydrogels are attractive materials with structures and functional properties similar to biological tissues and widely used in biomedical engineering. However, traditional synthetic hydrogels possess poor mechanical strength, and their applications are limited. Herein, a multidimensional material design method is developed; it includes the in situ gelation of silk fabric and nacre-inspired layer-by-layer assembly, which is used to prepare silk fibroin (SF) hydrogels. The in situ gelation method of silk fabric introduces a directionally ordered fabric network in a silk substrate, considerably enhancing the strength of hydrogels. Based on the nacre structure, the layer-by-layer assembly method enables silk hydrogels to break through the size limit and increase the thickness, realizing the longitudinal extension of the hydrogels. The application of the combined biomineralization and hot pressing method can effectively reduce interface defects and improve the interaction between organic and inorganic interfaces. The multidimensional material design method helps increase the strength (287.78 MPa), toughness (18.43 MJ m-3), and fracture energy (50.58 kJ m-2) of SF hydrogels; these hydrogels can weigh 2000 times their own weight. Therefore, SF hydrogels designed using the aforementioned combined method can realize the combination of strength and toughness and be used in biological tissue engineering and structural materials.

The energy dissipation property in bioinspired staggered composites with the viscoelastic matrix.

Many biological materials, such as bone and nacre, exhibit remarkable combinations of stiffness, strength, toughness, and impact resistance over millions of years of evolution. They provide prototypes for designing high-performance artificial composites. However, the dynamic properties of biological materials under impact loading are still not clear. In this study, we establish a dynamic shear-lag model to explore the dynamic response and the energy dissipation capacity of bioinspired staggered composites with a viscoelastic matrix under impact loading. The time domain solution of the dynamic shear-lag model is derived. Then, the model is verified by comparing it with the results from the finite element method. The results demonstrate that matrix viscosity plays a significant role in dissipating the impact energy and enhances the wave transformation between adjacent tablets. Furthermore, there exists an optimal viscosity coefficient to achieve an excellent balance between the rate and efficiency of energy dissipation. The model and the results can not only reveal the energy dissipation property of biological materials but also provide guidelines for the design and optimization of high-performance composites.

Nacre-mimetic cerium-doped nano-hydroxyapatite/chitosan layered composite scaffolds regulate bone regeneration via OPG/RANKL signaling pathway.

Autogenous bone grafting has long been considered the gold standard for treating critical bone defects. However, its use is plagued by numerous drawbacks, such as limited supply, donor site morbidity, and restricted use for giant-sized defects. For this reason, there is an increasing need for effective bone substitutes to treat these defects. Mollusk nacre is a natural structure with outstanding mechanical property due to its notable "brick-and-mortar" architecture. Inspired by the nacre architecture, our team designed and fabricated a nacre-mimetic cerium-doped layered nano-hydroxyapatite/chitosan layered composite scaffold (CeHA/CS). Hydroxyapatite can provide a certain strength to the material like a brick. And as a polymer material, chitosan can slow down the force when the material is impacted, like an adhesive. As seen in natural nacre, the combination of these inorganic and organic components results in remarkable tensile strength and fracture toughness. Cerium ions have been demonstrated exceptional anti-osteoclastogenesis capabilities. Our scaffold featured a distinct layered HA/CS composite structure with intervals ranging from 50 to 200 µm, which provided a conducive environment for human bone marrow mesenchymal stem cell (hBMSC) adhesion and proliferation, allowing for in situ growth of newly formed bone tissue. In vitro, Western-blot and qPCR analyses showed that the CeHA/CS layered composite scaffolds significantly promoted the osteogenic process by upregulating the expressions of osteogenic-related genes such as RUNX2, OCN, and COL1, while inhibiting osteoclast differentiation, as indicated by reduced TRAP-positive osteoclasts and decreased bone resorption. In vivo, calvarial defects in rats demonstrated that the layered CeHA/CS scaffolds significantly accelerated bone regeneration at the defect site, and immunofluorescence indicated a lowered RANKL/OPG ratio. Overall, our results demonstrate that CeHA/CS scaffolds offer a promising platform for bone regeneration in critical defect management, as they promote osteogenesis and inhibit osteoclast activation.

Calcitic Prisms of The Giant Seashell Pinna Nobilis Form Light Guide Arrays.

The shells of the Pinnidae family are based on a double layer of single-crystal-like calcitic prisms and inner aragonitic nacre, a structure known for its outstanding mechanical performance. However, on the posterior side, shells are missing the nacreous layer, which raises the question of whether there can be any functional role in giving up this mechanical performance. Here, it is demonstrated that the prismatic part of the Pinna nobilis shell exhibits unusual optical properties, whereby each prism acts as an individual optical fiber guiding the ambient light to the inner shell cavity by total internal reflection. This pixelated light channeling enhances both spatial resolution and contrast while reducing angular blurring, an apt combination for acute tracking of a moving object. These findings offer insights into the evolutionary aspects of light-sensing and imaging and demonstrate how an architectured optical system for efficient light-tracking can be based on birefringent ceramics.

Mussel- and nacre-inspired dual-bionic alginate-based hydrogel coating with multi-matrix applicability, high separation stability and antifouling performance for oil/water separation.

Natural hydrogel-modified porous matrices with superwetting interfaces are ideal for oil/water separation. In this study, inspired by two marine organisms, a novel hydrogel coating with multi-matrix suitability, high oil/water separation capability and antifouling properties was developed. Specifically, inspired by mussel byssus, hydrogel coating was successfully deposited on porous matrix surface based on the introduction of tannic acid (TA). Moreover, inspired by the "brick and mortar" microstructure of Pinctada nacre, silica particles were in-situ synthesized in the sodium alginate (SA)/Ca2+ hydrogel to provide the filling effect and to increase strength. Furthermore, Sodium alginate-tannic acid-tetraethyl orthosilicate (SA-TA-TEOS) hydrogel coating-modified membrane exhibited super-hydrophilic and underwater super-oleophobic performance (underwater oil contact angle >150°), and achieved efficient oil/water separation for four oil/water emulsions (flux = 493-584 L·m-2·h-1 and rejection = 97.3-99.5 %). The modified membrane also demonstrated good anti-fouling performance and flux recovery. Notably, hydrogel coating-modified non-woven fabric also had high oil/water separation capacity (rejection >98 %) and cyclic stability, which proved the universal applicability of this hydrogel coating. In short, this work provides new insights into the fabrication of hydrogel coating-modified porous materials based upon a marine organism biomimetic strategy, which has potential applications in separating oil/water emulsions in industrial scenarios.

miR-10a-3p Participates in Nacre Formation in the Pearl Oyster Pinctada fucata martensii by Targeting NPY.

MicroRNAs (miRNAs) are small noncoding RNAs that regulate gene expression via the recognition of their target messenger RNAs. MiR-10a-3p plays an important role in the process of ossification. In this study, we obtained the precursor sequence of miR-10a-3p in the pearl oyster Pinctada fucata martensii (Pm-miR-10a-3p) and verified its sequence by miR-RACE technology, and detected its expression level in the mantle tissues of the pearl oyster P. f. martensii. Pm-nAChRsα and Pm-NPY were identified as the potential target genes of Pm-miR-10a-3p. After the over-expression of Pm-miR-10a-3p, the target genes Pm-nAChRsα and Pm-NPY were downregulated, and the nacre microstructure became disordered. The Pm-miR-10a-3p mimic obviously inhibited the luciferase activity of the 3' untranslated region of the Pm-NPY gene. When the interaction site was mutated, the inhibitory effect disappeared. Our results suggested that Pm-miR-10a-3p participates in nacre formation in P. f. martensii by targeting Pm-NPY. This study can expand our understanding of the mechanism of biomineralization in pearl oysters.

Direct control of shell regeneration by the mantle tissue in the pearl oyster Pinctada fucata.

Molluscs rapidly repair the damaged shells to prevent further injury, which is vital for their survival after physical or biological aggression. However, it remains unclear how this process is precisely controlled. In this study, we applied scanning electronic microscope and histochemical analysis to examine the detailed shell regeneration process in the pearl oyster Pinctada fucata. It was found that the shell damage caused the mantle tissue to retract, which resulted in relocation of the partitioned mantle zones with respect to their correspondingly secreting shell layers. As a result, the relocated mantle tissue dramatically altered the shell morphology by initiating de novo precipitation of prismatic layers on the former nacreous layers, leading to the formation of sandwich-like "prism-nacre-prism-nacre" structure. Real-time PCR revealed the up-regulation of the shell matrix protein genes, which was confirmed by the thermal gravimetric analysis of the newly formed shell. The increased matrix secretion might have led to the change of CaCO3 precipitation dynamics which altered the mineral morphology and promoted shell formation. Taken together, our study revealed the close relationship between the physiological activities of the mantle tissue and the morphological change of the regenerated shells.

A Molecular-Scale Understanding of Misorientation Toughening in Corals and Seashells.

Biominerals are organic-mineral composites formed by living organisms. They are the hardest and toughest tissues in those organisms, are often polycrystalline, and their mesostructure (which includes nano- and microscale crystallite size, shape, arrangement, and orientation) can vary dramatically. Marine biominerals may be aragonite, vaterite, or calcite, all calcium carbonate (CaCO3 ) polymorphs, differing in crystal structure. Unexpectedly, diverse CaCO3 biominerals such as coral skeletons and nacre share a similar characteristic: Adjacent crystals are slightly misoriented. This observation is documented quantitatively at the micro- and nanoscales, using polarization-dependent imaging contrast mapping (PIC mapping), and the slight misorientations are consistently between 1° and 40°. Nanoindentation shows that both polycrystalline biominerals and abiotic synthetic spherulites are tougher than single-crystalline geologic aragonite. Molecular dynamics (MD) simulations of bicrystals at the molecular scale reveal that aragonite, vaterite, and calcite exhibit toughness maxima when the bicrystals are misoriented by 10°, 20°, and 30°, respectively, demonstrating that slight misorientation alone can increase fracture toughness. Slight-misorientation-toughening can be harnessed for synthesis of bioinspired materials that only require one material, are not limited to specific top-down architecture, and are easily achieved by self-assembly of organic molecules (e.g., aspirin, chocolate), polymers, metals, and ceramics well beyond biominerals.