A Stretchable and Tough Graphene Film Enabled by Mechanical Bond

The pursuit of fabricating high‐performance graphene films has aroused considerable attention due to their potential for practical applications. However, developing both stretchable and tough graphene films remains a formidable challenge. To address this issue, we herein introduce mechanical bond to comprehensively improve the mechanical properties of graphene films, utilizing [2]rotaxane as the bridging unit. Under external force, the [2]rotaxane cross‐link undergoes intramolecular motion, releasing hidden chain and increasing the interlayer slip distance between graphene nanosheets. Compared with graphene films without [2]rotaxane cross‐linking, the presence of mechanical bond not only boosted the strength of graphene films (247.3 vs 74.8 MPa) but also markedly promoted the tensile strain (23.6 vs 10.2 %) and toughness (23.9 vs 4.0 MJ/m3). Notably, the achieved tensile strain sets a record high and the toughness surpasses most reported results, rendering the graphene films suitable for applications as flexible electrodes. Even when the films were stretched within a 20 % strain and repeatedly bent vertically, the light‐emitting diodes maintained an on‐state with little changes in brightness. Additionally, the film electrodes effectively actuated mechanical joints, enabling uninterrupted grasping movements. Therefore, the study holds promise for expanding the application of graphene films and simultaneously inspiring the development of other high‐performance two‐dimensional films. A [2]rotaxane‐bridged graphene (RBG) film was fabricated, in which graphene nanosheets were cross‐linked by mechanical bonds. During the stretching process, the intramolecular motion of [2]rotaxanes resulted in the release of hidden chains, so that the mechanical properties of RBG films were improved, realizing the effect of strengthening and toughening graphene films.