Graphene nanoribbons present intriguing electronic properties due to their characteristic size and edge shape, and have been suggested for a wide range of applications from electronics to electromechanical systems. To bridge the scales from their nanostructural geometry—the key for their unique properties—to the requirements critical for large-scale electronics and device applications, here we propose a de novo hierarchical material assembled from functionalized graphene nanoribbons stabilized through hydrogen bonds, mimicking the structure of beta-sheet proteins. By investigating their mechanical and electronic properties through first principles calculations, we demonstrate that hierarchical graphene nanoribbons not only preserve the unique electronic properties of individual graphene nanoribbons in the bulk, but are also energetically and mechanically stable. Specifically, we find that the energy gap of the bulk material shrinks as the width of the constituting graphene nanoribbons increases. The tuning of bulk material properties through controlling the nanostructure enables the synthesis of a broader class of biomimetic multifunctional mechanomutable and electromutable nanomaterials for electromechanical applications.