Crumpled graphene films are widely used, for instance in electronics1, energy storage2,3, composites4,5 and biomedicine6. Although it is known that the degree of crumpling affects graphene’s properties and the performance of graphene-based devices and materials3,5,7, the controlled folding and unfolding of crumpled graphene films has not been demonstrated. Here we report an approach to reversibly control the crumpling and unfolding of large-area graphene sheets. We show with experiments, atomistic simulations and theory that, by harnessing the mechanical instabilities of graphene adhered on a biaxially pre-stretched polymer substrate and by controlling the relaxation of the pre-strains in a particular order, graphene films can be crumpled into tailored self-organized hierarchical structures that mimic superhydrophobic leaves. The approach enables us to fabricate large-area conductive coatings and electrodes showing superhydrophobicity, high transparency, and tunable wettability and transmittance. We also demonstrate that crumpled graphene–polymer laminates can be used as artificial-muscle actuators.
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The research is primarily funded by the NSF’s Research Triangle MRSEC (DMR-1121107), NSF (CMMI-1200515) and NIH (UH2 TR000505). X.Z. acknowledges the support from the Pratt School of Engineering Seed Grant. S.R. and M.J.B. acknowledge the support from AFOSR (FA9550-11-1-0199) and NSF-MRSEC (DMR-0819762). M.J.B. and N.P. acknowledge the support from the MIT-Italy Program (MITOR). N.P. acknowledges the support from the European Research Council under the European Union’s Seventh Framework Programme (FP7/2007–2013)/ERC Grant agreement number  (ERC StG Ideas 2011 BIHSNAM). J.Z. and X.Z. acknowledge the help from C-H. Chen on contact-angle measurements and B. Wiley on transmittance measurements.
The authors declare no competing financial interests.
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Zang, J., Ryu, S., Pugno, N. et al. Multifunctionality and control of the crumpling and unfolding of large-area graphene. Nature Mater 12, 321–325 (2013). https://doi.org/10.1038/nmat3542
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