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The electroactivity as a supramolecular feature of intelligently designed self-assembled systems stimulates a wide interest in development of new stimuli-responsive biomaterials. A diverse set of nanostructures are fabricated through programmed self-assembly of molecules for functional materials. Electroactive groups are conjugated as a functional moiety for organic semiconductor applications. In this review, we present recent examples of self-assembling peptide molecules and electroactive units for supramolecular functional electronic ​and optical materials with potential biomedical and bioelectronics applications.