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Clasping folds enable superior elastic strength of graphene films

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References

  1. Lee, C., Wei, X., Kysar, J. W. & Hone, J. Measurement of the elastic properties and intrinsic strength of monolayer graphene. Science 321, 385–388 (2008).

    Article  CAS  PubMed  Google Scholar 

  2. Golberg, D. et al. Boron nitride nanotubes and nanosheets. ACS Nano 4, 2979–2993 (2010).

    Article  CAS  PubMed  Google Scholar 

  3. Nicolosi, V., Chhowalla, M., Kanatzidis, M. G., Strano, M. S. & Coleman, J. N. Liquid exfoliation of layered materials. Science 340, 1226419 (2013).

    Article  Google Scholar 

  4. Lipatov, A. et al. Elastic properties of 2D Ti3C2Tx MXene monolayers and bilayers. Sci. Adv. 4, eaat0491 (2018).

    Article  PubMed  PubMed Central  Google Scholar 

  5. Tan, C. L. et al. Recent advances in ultrathin two dimensional nanomaterials. Chem. Rev. 117, 6225–6331 (2017).

    Article  CAS  PubMed  Google Scholar 

  6. Li, Y., Lian, W. & Cheng, Q. High-performance nacre-inspired 2D carbon-based nanocomposites. Adv. Mater. 37, 2501932 (2025).

    Article  CAS  Google Scholar 

  7. Putz, K. W. et al. Evolution of order during vacuum-assisted self-assembly of graphene oxide paper and associated polymer nanocomposites. ACS Nano 5, 6601–6609 (2011).

    Article  CAS  PubMed  Google Scholar 

  8. Zhong, J. et al. Efficient and scalable synthesis of highly aligned and compact two-dimensional nanosheet films with record performances. Nat. Commun. 9, 3484 (2018).

    Article  PubMed  PubMed Central  Google Scholar 

  9. Li, P. et al. Continuous crystalline graphene papers with gigapascal strength by intercalation modulated plasticization. Nat. Commun. 11, 2645 (2020).

    Article  CAS  PubMed  PubMed Central  Google Scholar 

  10. Zhao, C. et al. Layered nanocomposites by shear-flow-induced alignment of nanosheets. Nature 580, 210–215 (2020).

    Article  CAS  PubMed  Google Scholar 

  11. Yang, J. et al. Water-induced strong isotropic MXene-bridged graphene sheets for electrochemical energy storage. Science 383, 771–777 (2024).

    Article  CAS  PubMed  Google Scholar 

  12. Patil, V. P., Sandt, J. D., Kolle, M. & Dunkel, J. Topological mechanics of knots and tangles. Science 367, 71–75 (2020).

    Article  MathSciNet  CAS  PubMed  Google Scholar 

  13. Jawed, M. K., Dieleman, P., Audoly, B. & Reis, P. M. Untangling the mechanics and topology in the frictional response of long overhand elastic knots. Phys. Rev. Lett. 115, 118302 (2015).

    Article  CAS  PubMed  Google Scholar 

  14. Zhou, T. et al. Super-tough MXene-functionalized graphene sheets. Nat. Commun. 11, 2077 (2020).

    Article  CAS  PubMed  PubMed Central  Google Scholar 

  15. Kim, S. M. et al. Synthesis of large-area multilayer hexagonal boron nitride for high material performance. Nat. Commun. 6, 8662 (2015).

    Article  CAS  PubMed  PubMed Central  Google Scholar 

  16. Podsiadlo, P. et al. Ultrastrong and stiff layered polymer nanocomposites. Science 318, 80–83 (2007).

    Article  CAS  PubMed  Google Scholar 

  17. Bonderer, L. J., Studart, A. B. & Gauckler, L. J. Bioinspired design and assembly of platelet reinforced polymer films. Science 319, 1069–1073 (2008).

    Article  CAS  PubMed  Google Scholar 

  18. Tang, Z. Y., Kotov, N. A., Magonov, S. & Ozturk, B. Nanostructured artificial nacre. Nat. Mater. 2, 413–418 (2003).

    Article  CAS  PubMed  Google Scholar 

  19. Kakisawa, H. & Sumitomo, T. The toughening mechanism of nacre and structural materials inspired by nacre. Sci. Technol. Adv. Mater. 12, 064710 (2011).

    Article  PubMed  Google Scholar 

  20. Gao, H., Ji, B., Jäger, I. L., Arzt, E. & Fratzl, P. Materials become insensitive to flaws at nanoscale: lessons from nature. Proc. Natl Acad. Sci. USA 100, 5597–5600 (2003).

    Article  CAS  PubMed  PubMed Central  Google Scholar 

  21. Ji, B. & Gao, H. Mechanical principles of biological nanocomposites. Annu. Rev. Mater. Res. 40, 77–100 (2010).

    Article  CAS  Google Scholar 

  22. Liu, Y., Xie, B., Zhang, Z., Zheng, Q. & Xu, Z. Mechanical properties of graphene papers. J. Mech. Phys. Solids 60, 591–605 (2012).

    Article  MathSciNet  CAS  Google Scholar 

  23. Wang, S., Lin, J., Xu, Z. & Xu, Z. Understanding macroscopic assemblies of carbon nanostructures with microstructural complexity. Compos. Part A 143, 106318 (2021).

    Article  CAS  Google Scholar 

  24. Zhao, H., Yang, Z. & Guo, L. Nacre-inspired composites with different macroscopic dimensions: strategies for improved mechanical performance and applications. NPG Asia Mater. 10, 1–22 (2018).

    Article  Google Scholar 

  25. Yang, M. & Kotov, N. A. Quantitative biomimetics of high-performance materials. Nat. Rev. Mater. 10, 382–395 (2025).

    Article  CAS  Google Scholar 

  26. Wan, S., Fang, S., Jiang, L., Cheng, Q. & Baughman, R. H. Strong, conductive, foldable graphene sheets by sequential ionic and π bridging. Adv. Mater. 30, 1802733 (2018).

    Article  Google Scholar 

  27. Wang, L. et al. Superior strong and tough nacre-inspired materials by interlayer entanglement. Nano Lett. 23, 3352–3361 (2023).

    Article  CAS  PubMed  Google Scholar 

  28. Wan, S. et al. Scalable ultrastrong MXene films with superior osteogenesis. Nature 634, 1103–1110 (2024).

    Article  CAS  PubMed  Google Scholar 

  29. Hummers, W. S. & Offeman, R. E. Preparation of graphitic oxide. J. Am. Chem. Soc. 80, 1339 (1958).

    Article  CAS  Google Scholar 

  30. Dreyer, D. R., Park, S., Bielawski, C. W. & Ruoff, R. S. The chemistry of graphene oxide. Chem. Soc. Rev. 39, 228–240 (2010).

    Article  CAS  PubMed  Google Scholar 

  31. Ferrari, A. C. et al. Raman spectrum of graphene and graphene layers. Phys. Rev. Lett. 97, 187401 (2006).

    Article  CAS  PubMed  Google Scholar 

  32. Giudice, F. & Shen, A. Shear rheology of graphene oxide dispersions. Curr. Opin. Chem. Eng. 16, 23–30 (2017).

    Article  Google Scholar 

  33. Xiong, Z. et al. Ultrahigh concentration exfoliation and aqueous dispersion of few-layer graphene by excluded volume effect. Nat. Commun. 15, 10807 (2024).

    Article  PubMed  PubMed Central  Google Scholar 

  34. Juan, J., Nó, M. & Schuh, C. Nanoscale shape-memory alloys for ultrahigh mechanical damping. Nat. Nanotechnol. 4, 415–419 (2009).

    Article  Google Scholar 

  35. Wang, R. Z., Suo, Z., Evans, A. G., Yao, N. & Aksay, I. A. Deformation mechanisms in nacre. J. Mater. Res. 16, 2485–2493 (2001).

    Article  CAS  Google Scholar 

  36. Jackson, A. P., Vincent, J. F. V. & Turner, R. M. The mechanical design of nacre. Proc. R. Soc. Lond. B 234, 415–440 (1988).

    Article  Google Scholar 

  37. Pan, X. F. et al. Recyclable nacre-like aramid-mica nanopapers with enhanced mechanical and electrical insulating properties. Adv. Funct. Mater. 33, 2210901 (2023).

    Article  CAS  Google Scholar 

  38. Shen, K. et al. Intercalated oligomer doubles plasticity for strong and conductive graphene papers and composites. Carbon 208, 160–169 (2023).

    Article  CAS  Google Scholar 

  39. Zhou, T. et al. Ultratough graphene-black phosphorus films. Proc. Natl Acad. Sci. USA 117, 8727–8735 (2020).

    Article  CAS  PubMed  PubMed Central  Google Scholar 

  40. Xiao, Y. et al. Sheet collapsing approach for rubber-like graphene papers. ACS Nano 11, 8092–8102 (2017).

    Article  CAS  PubMed  Google Scholar 

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Acknowledgements

We thank X. Zhang for assistance with AFM measurements; G. Zhu and Q. Lin for assistance with TEM measurements; and Y. Qiu for help in conducting SAXS and wide-angle X-ray scattering measurements.

Funding

This work was financially supported by the National Key Research and Development Program of China (2022YFA1205300 and 2022YFA1205301), the National Natural Science Foundation of China (52122301, 52090030, 52090031, 52090032, 52502120, 52272046, 12425201 and 52302049), the ‘Pioneer’ and ‘Leading Goose’ R&D Program of Zhejiang (2023C01190 and 2026C02A1055), the Fundamental Research Funds for the Central Universities (226-2024-00074 and 226-2025-00219), the Space Application System of China Manned Space Program (CMSS-2024-4-A-013) and the National Key Basic Research Program of China through grant (2022YFA1205400). Computation was performed on the Explorer 1000 cluster system of the Tsinghua National Laboratory for Information Science and Technology.

Author information

Author notes

  1. These authors contributed equally: Lidan Wang, Yangchao Liao

Authors and Affiliations

  1. MOE Key Laboratory of Macromolecular Synthesis and Functionalization, International Research Center for X Polymers, Zhejiang Key Laboratory of Advanced Organic Materials and Technologies, Research Center for Advanced Fibers, Department of Polymer Science and Engineering, Zhejiang University, Hangzhou, China

    Lidan Wang, Chenwei Shen, Lu Chen, Mingtao Zhang, Kaiwen Li, Peng Li, Yingjun Liu, Zhen Xu, Kai Pang & Chao Gao

  2. Applied Mechanics Laboratory, Department of Engineering Mechanics and Center for Nano and Micro Mechanics, Tsinghua University, Beijing, China

    Yangchao Liao, Jingjie Huang & Zhiping Xu

  3. School of Civil and Environment Engineering, Changsha University of Science and Technology, Changsha, China

    Yangchao Liao

  4. State Key Laboratory of Silicon and Advanced Semiconductor Materials and School of Materials Science & Engineering, Zhejiang University, Hangzhou, China

    Xing Li & Degong Ding

  5. Institute of Physics, Chinese Academy of Sciences, Beijing, China

    Li Peng

Authors

  1. Lidan Wang
  2. Yangchao Liao
  3. Jingjie Huang
  4. Chenwei Shen
  5. Lu Chen
  6. Xing Li
  7. Degong Ding
  8. Mingtao Zhang
  9. Li Peng
  10. Kaiwen Li
  11. Peng Li
  12. Yingjun Liu
  13. Zhen Xu
  14. Kai Pang
  15. Zhiping Xu
  16. Chao Gao

Contributions

L.W., Zhen Xu, K.P., Zhiping Xu and C.G. supervised the project. L.W. made the initial key finding. L.W., K.P. and Zhen Xu conceived the idea and designed the experiments. L.W., K.P. and Zhen Xu performed the experiments and characterizations. C.S., L.C., L.P. and K.L. assisted with AFM and TEM characterizations. D.D. and X.L. performed the in-situ TEM tensile experiments. M.Z. contributed to the analysis of SFGO nanosheet preparation. P.L. and Y. Liu assisted in FIB characterization. Y. Liao, J.H. and Zhiping Xu performed the theoretical analysis. L.W. wrote the initial draft of the manuscript, and L.W., Zhen Xu, K.P., Zhiping Xu and C.G. revised it. All authors discussed the results and approved the final version of the paper.

Corresponding authors

Correspondence to Zhen Xu, Kai Pang, Zhiping Xu or Chao Gao.

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Competing interests

The authors declare no competing interests.

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Extended data figures and tables

Extended Data Fig. 1 AFM analyses of surface folds of SFGOs.

a, Photo of GO dispersion (0.1 mg ml−1) and its AFM image, height profile, 3D surface morphology (from top). b, Photos of dispersions (0.1 mg ml−1) and AFM images, height profiles, 3D surface morphologies (from top) for four SFGOs samples synthesized at decreased temperature: SFGO-1 (−5 °C), SFGO-2 (−10 °C), SFGO-3 (−15 °C) and SFGO-4 (−25 °C). The synthesis processes of four SFGO samples see details in Supplementary Experimental Section. c, The thickness of SFGO flakes as a function of reaction temperature. Data are presented as mean ± standard deviation (n = 30 independent samples). d, The fold width and length for four SFGO samples, statistically calculated from AFM analyses (b). e, Fold density for SFGO samples and GO.

Source data

Extended Data Fig. 2 Characterizations of lamellar crystallinity of SFGOs.

a, On-site photo of XRD testing for SFGO dispersion samples. b, XRD patterns of graphite, GO and SFGOs dispersions (at 20 mg ml−1). c,d, AC-TEM images of surface folds (c) and the stacking moiré pattern on planar surface (d) of SFGO-1 flake. e, Raman spectra of graphite, GO, SFGO-1, SFGO-2, SFGO-3 and SFGO-4. f, The ID/IG value and C/O ratio as a function of reaction temperature. ID/IG data are presented as mean ± standard deviation (n = 3 independent samples).

Source data

Extended Data Fig. 3 Raman analyses on the heterogeneous core-shell structure of SFGO.

a, The schematic process for sample preparation and Raman testing for a SFGO-4 flake. b,c, Typical Raman spectra collecting on surface (b) and core (c). d, The ID/IG distribution on surface and core by randomly selected 10 samplings. Data are presented as mean ± standard deviation (n = 10 independent samples).

Source data

Extended Data Fig. 4 TEM images and structural models.

a, RG film features some wrinkles on sheets. b, SFRG-1 film exhibits typical FCL structure. c, SFRG-4 film contains large voids and gaps, resulted by the  nonuniform stacking of intrinsically thick flakes.

Extended Data Fig. 5 Preparation and structural characterization of SFGO film.

a, Photograph of blade coating SFGO film. Scale bar, 10 cm. b,c, XRD patterns of SFGO-1 and GO film before (b) and after reduction (c). d, The corresponding interlayer spacing and grain size of SFRG-1 and RG film calculated from XRD spectra. e, Raman spectra of SFGO-1, SFRG-1, GO and RG film. f, WAXS patterns and azimuthal scan profiles (002 peak) of the SFRG-1 and RG film. WAXS patterns were recorded along the parallel direction with an incident Cu-Kα X-ray beam. g, XPS analyses of SFGO-1 and SFRG-1 film. h,i, The C1s spectra of SFGO-1 (h) and SFRG-1 (i) film. The broad C1s peak of SFGO films was fitted by three peaks at 284.3, 286.3, and 288.0 eV, corresponding to C(sp2)-C(sp2), C-O, and C-O-C, respectively. The proportion of C(sp2)-C(sp2) (57.9%) for SFGO films increased to 87.8% for SFRG film, indicating the substantial elimination of oxygen-containing groups of SFGO flakes by chemical reduction.

Source data

Extended Data Fig. 6 In-situ WAXS characterization of the elasticity in SFRG-1 film.

a, In-situ WAXS testing apparatus. b, WAXS patterns for the 002 peak of the SFRG-1 film during the loading (up) and unloading (down). c,d, Azimuthal scan profiles for the 002 peak during loading (c) and unloading (d). e, The degree of orientation of the SFRG-1 films as a function of elongation during loading and unloading process.

Source data

Extended Data Fig. 7 Configurations, stress distributions, and strain distributions of the single-layer folded GO model with W = 50 nm.

a, The three typical states of the system during the tensile process: the initial state, the maximum-stress state, and the interlayer interlock failure state. Here, W represents the width of a single fold, L0 = 360 nm denotes the initial length used to calculate the engineering strain ε = (L – L0) / L0, and L represents the span between loading points. b, Configurations, stress distributions, and strain distributions of the head-to-head zone indicated by the blue-dashed box in panel a during the tensile process. c, Configurations, stress distributions, and strain distributions of the head-to-tail zone indicated by the red dashed box in panel a during the tensile process.

Extended Data Fig. 8

Tensile curves obtained from experiments, and fitted to the “pull-to-push” and the “shear-lag” models under the same parameters, respectively.

Source data

Supplementary information

Source data

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Wang, L., Liao, Y., Huang, J. et al. Clasping folds enable superior elastic strength of graphene films. Nature 658, 643–649 (2026). https://doi.org/10.1038/s41586-026-11109-y

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