Nature builds proteins out of particular molecular sequences to achieve specific functions, while human manufactured polymeric materials are often involving just one or two molecules. Developing routes to use de novo designed peptides and polymers as building blocks and manipulate their assemblage, should allow us to not only mimic nature, but also construct functional biomolecular materials with non-proceeding performances.

I will discuss the development of designed amphiphilic 4-helix bundle peptides derived from natural photosynthesis proteins and the manipulation of their applications on controlling the vectorial orientation and local environment of extended conjugated chromophores, as well as assembling the peptides into macroscopic functional biomaterial in Langmuir monolayer and the nanoporous films toward light harvesting. In addition, I will discuss a new design of peptide-polymer conjugates where a polymer chain is covalently linked to the side chain of a helical bundle-forming peptide. The effect of conjugated polymer chains on the peptide structures was examined using a de novo designed 3-helix bundle and a photoactive 4-helix bundle. Upon attachment of poly(ethylene glycol) (PEG) to the exterior of the coiled-coil helical bundle, the peptide secondary structure was stabilized and the tertiary structure, i.e. the coiled-coil helical bundle, was retained. Using a photoactive heme-binding 4-helix bundle-forming peptide as an example, the new peptide-polymer conjugate architecture also preserves the built-in functionalities within the interior of the helix bundle. The conjugated polymer chains on the exterior of the helix bundle will mediate the interactions between the helix bundle and its external environment. Thus, this new peptide-polymer conjugate design strategy not only opens new avenues to macroscopically assemble the helix bundles, but enable them to function in non-biological environments.