Eleonora Cataldi, Martina Raschig, Marcus Gutmann, Patrick T. Geppert, Matthias Ruopp, Marvin Schock, Hubert Gerwe, Rüdiger Bertermann, Lorenz Meinel, Maik Finze, Agnieszka Nowak‐Król, Michael Decker, Tessa Lühmann

• The incorporation of photoswitches into the molecular structure of peptides and proteins enables their dynamic photocontrol in complex biological systems. Here, a perfluorinated azobenzene derivative triggered by amber light was site‐specifically conjugated to cysteines in a helical peptide by perfluoroarylation chemistry. In response to the photoisomerization (trans→cis) of the conjugated azobenzene with amber light, the secondary structure of the peptide was modulated from a disorganized into an amphiphilic helical structure.