The engineering of supramolecular assemblies at the molecular level to achieve a specific function has been a longstanding challenge in various fields that utilizes bottom-up self-assembly strategies. We present a coassembled pi-conjugated peptide system composed of oligo-(p-phenylenevinylene)-based donor units and quaterthiophene-based acceptor units that demonstrate energy transfer in completely aqueous environments. The formation of one-dimensional nanostructures by the peptide assemblies bearing semiconducting units encourages energy migration along the stacking axis, thus resulting in the quenching of donor emission peaks along with the development of new spectral features reminiscent of acceptor emission. The effect of environmental stimuli (pH, temperature) to nanostructure formation and energy transfer will also be presented. To further emphasize the ability of these peptide-pi-peptide constructs to have rationally designed properties, the study on the sequence-dependent photophysical, rheological, and electrical properties of these semiconducting peptide hydrogelators will be presented. This aspect demonstrates the effects of amino acid sequence on the nanoscale to the macroscale electrical transport and mechanical properties of nanostructure-forming pi-conjugated peptides. Overall, this unique material design that can coassemble two different semiconducting units within peptide nanostructures and have sequence-tunable properties offers a new platform for the engineering of energy transport through bioelectronic materials in aqueous environments.