We present a new design of peptide-polymer conjugates where a polymer chain is covalently linked to the side chain of a helix bundle-forming peptide.The effect of conjugated polymer chains on the peptide structure was examined using a de novo designed three-helix bundle and a photoactive four-helix bundle.Upon attachment of poly(ethylene glycol)to the exterior of the coiled-coil helix bundle,the peptide secondary structure was stabilized and the tertiary structure,that is,the coiled-coil helix bundle,was retained.When a heme-binding peptide as an example is used,the new peptide-polymer conjugate architecture also preserves the built-in functionalities within the interior of the helix bundle.It is expected that the conjugated polymer chains act to mediate the interactions between the helix bundle and its external environment.Thus,this new peptide-polymer conjugate design strategy may open new avenues to macroscopically assemble the helix bundles and may enable them to function in nonbiological environments.
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