Polyethylene terephthalate (PET) is the most widely used polymer in the world. For the first time, the laser‐driven integration of aluminum nanoparticles (Al NPs) into PET to realize a laser‐induced graphene/Al NPs/polymer composite, which demonstrates excellent toughness and high electrical conductivity with the formation of aluminum carbide into the polymer is shown. The conductive structures show an impressive mechanical resistance against >10000 bending cycles, projectile impact, hammering, abrasion, and structural and chemical stability when in contact with different solvents (ethanol, water, and aqueous electrolytes). Devices including thermal heaters, carbon electrodes for energy storage, electrochemical and bending sensors show this technology's practical application for ultra‐robust polymer electronics. This laser‐based technology can be extended to integrating other nanomaterials and create hybrid graphene‐based structures with excellent properties in a wide range of flexible electronics’ applications.

We show a novel concept for the design of graphene-based materials via diazonium-mediated functionalization and subsequent laser treatment for flexible electronics.

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