The use of graphene in a form of discontinuous flakes in polymer composites limits the full exploitation of the unique properties of graphene, thus requiring high filler loadings for achieving- for example- satisfactory electrical and mechanical properties. Herein centimetre-scale CVD graphene/polymer nanolaminates have been produced by using an iterative ‘lift-off/float-on’ process and have been found to outperform, for the same graphene content, state-of-the-art flake-based graphene polymer composites in terms of mechanical reinforcement and electrical properties. Most importantly these thin laminate materials show a high electromagnetic interference (EMI) shielding effectiveness, reaching 60 dB for a small thickness of 33 μm, and an absolute EMI shielding effectiveness close to 3·105 dB cm2 g−1 which is amongst the highest values for synthetic, non-metallic materials produced to date.

Graphene is susceptible to morphological instabilities such as wrinkles and folds, which result from the imposition of thermo-mechanical stresses upon cooling from high temperatures and/ or under biaxial loading. A particular pattern encountered in CVD graphene is that of mosaic formation. Although it is understood that this pattern results from the severe biaxial compression upon cooling from high temperatures, it has not been possible to create such a complex pattern at room temperature by mechanical loading. Herein, we have managed by means of lateral wrinkling induced by tension and Euler buckling resulting from uniaxial compression upon unloading, to create such patterns in exfoliated graphene. We also show that these patterns can be used as channels for trapping or administering fluids at interstitial space between graphene and its support. This opens a whole dearth of new applications in the area of nano-fluidics but also in photo-electronics and sensor technologies.

Wrinkles in supported graphenes can be formed either by uniaxial compression or uniaxial tension beyond a certain critical load depending on the mode of loading. In the first case, the wrinkling direction is normal to the compression axis whereas in tension, wrinkles of the same pattern are formed parallel to the loading direction due to Poisson's (lateral) contraction. Herein we show by direct AFM observations that in simply-supported graphenes such instabilities appear as periodic wrinkles over existing stochastic undulations caused by the underlying-substrate-roughness. The critical strain for the generation of these wrinkles in both tension and compression is less than 1% which particularly for the former is far lower than the predicted tensile strain to fracture of suspended graphene estimated at ∼30%. Based on these findings, a constitutive model that provides the critical tensile strain for induced buckling in the lateral direction is proposed that depends only on the graphene-support interaction and not on the nature of the substrate. Understanding the wrinkling failure of graphenes under strain is of paramount importance as it leads to new threshold limits beyond which the physical-mechanical properties of graphene are impaired.