This work describes a strategy to create terthiophene (3T)-naphthalenediimide (NDI) nanostructures via the beta-sheet self-assembly of a functionalized dipeptide. The dipeptide assembles into 1D nanofibers in organic solvents and forms a self-supporting organogel at low concentrations in CH2Cl2. The nanostructures engage in extensive intermolecular pi-pi stacking interactions.