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It is unavoidable to form wrinkles, which are folds or creases in a material, in graphene, whenever the graphene is prepared by micromechanical exfoliation from graphite or chemical vapor deposition (CVD). However, the controllable formation and structures of graphene with nanoscale wrinkles remains a big challenge. Here, we report a liquid-phase shrink method to controllably fabricate large area wrinkled graphene (WG). The CVD-prepared graphene self-shrinks into a WG on an ethanol solution surface. By modifying the concentration of the ethanol solution, we can easily and efficiently obtain WG with a uniform distribution of wrinkles with different heights. The WG shows high stretchability and can withstand more than 100% tensile strain and up to 720 degrees twist. Furthermore, electromechanical response sensors based on double-layer stacking of WG show ultrahigh sensitivity. This simple, effective, and environmentally friendly liquid-phase shrink method will pave a way for the controllable formation of WG, which is an ideal candidate for application in highly stretchable and highly sensitive electronic devices.

It is unavoidable to form wrinkles, which are folds or creases in a material, in graphene, whenever the graphene is prepared by micromechanical exfoliation from graphite or chemical vapor deposition (CVD). However, the controllable formation and structures of graphene with nanoscale wrinkles remains a big challenge. Here, we report a liquid-phase shrink method to controllably fabricate large area wrinkled graphene (WG). The CVD-prepared graphene self-shrinks into a WG on an ethanol solution surface. By modifying the concentration of the ethanol solution, we can easily and efficiently obtain WG with a uniform distribution of wrinkles with different heights. The WG shows high stretchability and can withstand more than 100% tensile strain and up to 720 degrees twist. Furthermore, electromechanical response sensors based on double-layer stacking of WG show ultrahigh sensitivity. This simple, effective, and environmentally friendly liquid-phase shrink method will pave a way for the controllable formation of WG, which is an ideal candidate for application in highly stretchable and highly sensitive electronic devices.

It is unavoidable to form wrinkles, which are folds or creases in a material, in graphene, whenever the graphene is prepared by micromechanical exfoliation from graphite or chemical vapor deposition (CVD). However, the controllable formation and structures of graphene with nanoscale wrinkles remains a big challenge. Here, we report a liquid-phase shrink method to controllably fabricate large area wrinkled graphene (WG). The CVD-prepared graphene self-shrinks into a WG on an ethanol solution surface. By modifying the concentration of the ethanol solution, we can easily and efficiently obtain WG with a uniform distribution of wrinkles with different heights. The WG shows high stretchability and can withstand more than 100% tensile strain and up to 720 degrees twist. Furthermore, electromechanical response sensors based on double-layer stacking of WG show ultrahigh sensitivity. This simple, effective, and environmentally friendly liquid-phase shrink method will pave a way for the controllable formation of WG, which is an ideal candidate for application in highly stretchable and highly sensitive electronic devices.