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.

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Glass electronics inspire the emergence of smart functional surfaces. To evolve this concept to the next level, developing new strategies for scalable, inexpensive, and electrically conductive glass‐based robust nanocomposites is crucial. Graphene is an attractive material as a conductive filler; however, integrating it firmly into a glass with no energy‐intensive sintering, melting, or harsh chemicals has not been possible until now. Moreover, these methods have very limited capability for fabricating robust patterns for electronic circuits. In this work, a conductive (160 OΩ sq−1) and resilient nanocomposite between glass and graphene is achieved via single‐step laser‐induced backward transfer (LIBT). Beyond conventional LIBT involving mass transfer, this approach simultaneously drives chemical transformations in glass including silicon compound formation and graphene oxide (GO) reduction. These processes take place together with the generation and transfer of the highest‐quality laser‐reduced GO (rGO) reported to date (Raman intensity ratio ID/IG = 0.31) and its integration into the glass. The rGO‐LIBT nanocomposite is further functionalized with silver to achieve a highly sensitive (10−9 m) dual‐channel plasmonic optical and electrochemical sensor. Besides the electrical circuit demonstration, an electrothermal heater is fabricated that reaches temperatures above 300 °C and continuously operates for over 48 h.