Electrochemistry is emerging as a scalable and sustainable approach to organic synthesis. Nevertheless, applications of this powerful technique to the modification of complex biomolecules, such as peptides, are limited. We are interested in extending electro-organic synthesis to the preparation of designer peptides, including bioactive drug leads. The group has recently developed a method for the direct decarboxylative arylation of peptides. This project will explore additional opportunities for the efficient electrochemical modification of peptides, including through the use of novel “electrochemically-active” amino acids.