Early work with viologen‐mediated nitrogenase bio‐electrochemistry focused on bio‐electrocatalysis with the enzyme in solution, but biocatalyst immobilization at electrode surfaces is favorable as it provides a high effective concentration of biocatalyst at the electrode surface. We have used a pyrene–peptide linker as a method for immobilizing nitrogenase on carbon electrode surfaces for nitrogenase bio‐electrocatalysis.