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A variety of biomolecules such as peptides, carbohydrates, nucleobases, and nucleotides have been functionalized with the semiconducting organic π-conjugated systems for the synthesis of self-assembled nanostructures and their applications in supramolecular electronics. Among these biomolecules, peptides are one of the most attractive bio-segments for the self-assembly of π-conjugated systems (oligothiophenes, oligo(p-phenylenevinylenes) (OPVs), and perylene diimides (PDIs) because of their structural variability and the tendency to participate in non-covalent interactions viz. π-π stacking and hydrogen bonding. Therefore, peptide functionalized π-conjugated systems can provide the controlled assembly of π-conjugated units into highly ordered structures for effective charge-carrier mobility in supramolecular organic electronics. Moreover, among the variety of those π-conjugated chromophores, oligothiophenes are one of the most studied systems owing to their relatively high conductivity, chemical stability, solubility, and processability. In this presentation, I will highlight the current strategies to access nanostructured supramolecular assemblies of various π-conjugated peptides and detail their characterization using advanced spectroscopy and microscopy tools.