The development of complex self-assembling supramolecular systems derived from single, and sometimes simple, molecules has become an area of vast interest. These molecules are specifically designed to foster favorable intermolecular interactions leading to highly ordered macromolecular assemblies through 'bottom-up' fabrication with size dimensions that are on the order of nanometers to tens of microns. Self-assembling amyloid-like nanostructures provide biologically relevant systems that can be harnessed for the development of novel nanobiomaterials. Amyloid-like materials are composed of well-defined one dimensional (1-D) structures that can be used as scaffolding for controlled organization of organic electronic materials in aqueous environments. We have developed and functionalized a wide array of organic semiconductors and incorporated them into oligopeptides designed to self-assemble into 1-D amyloid-like nanofibers. These nanofibers have internalized intermolecularly delocalized pi-stacked oligothiophenes as well as linearly conjugated polydiacetylene (PDA) polymers running along the nanofiber long axis. These nanofibers can be globally aligned and fabricated into electronic devices that have a high degree of directionally dependent charge mobility. Preliminary experiments have also shown that these materials can be interfaced with biological systems with potential use as electro-active cell culture matrices.