Seriography‐Guided Reduction of Graphene Oxide Biopapers for Wearable Sensory Electronics

Novel nacre‐mimic bio‐nanocomposites, such as graphene‐based laminates, are pushing the boundaries of strength and toughness as flexible engineering materials. Translating these material advances to functional flexible electronics requires methods for generating print‐scalable microcircuits (conductive elements surrounded by dielectric) into these strong, tough, lightweight bio‐nanocomposites. Here, a new paradigm for printing flexible electronics by employing facile, eco‐friendly seriography to confine the reduction of graphene oxide biopapers reinforced by silk interlayers is presented. Well‐defined, micropatterned regions on the biopaper are chemically reduced, generating a 106 increase in conductivity (up to 104 S m−1). Flexible, robust graphene‐silk circuits are showcased in diverse applications such as resistive moisture sensors and capacitive proximity sensors. Unlike conductive (i.e., graphene‐ or Ag nanoparticle‐loaded) inks printed onto substrates, seriography‐guided reduction does not create mechanically weak interfaces between dissimilar materials and does not require the judicious formation of ink. The unimpaired functionality of printed‐in graphene‐silk microcircuits after thousands of punitive folding cycles and chemical attack by harsh solvents is demonstrated. This novel approach provides a low‐cost, portable solution for printing micrometer‐scale conductive features uniformly across large areas (>hundreds of cm2) in layered composites for applications including wearable health monitors, electronic skin, rollable antennas, and conformable displays. Robust, resilient, foldable microcircuits and sensors are printed in graphene‐silk biocomposite films by localizing the application of a reductant paste using a low‐cost screen printing setup. This approach provides a portable solution for the micropatterned reduction of graphene biopapers across large areas exceeding hundreds of cm2 for emerging applications in flexible electronics.