Efficient chemical modification of tryptophan (Trp) is of great interest because Trp and its analogues are widely found in many natural products and biomolecules such as peptides and proteins [1] and are important components for their biological activity. Therefore, the development of a new Trp-selective modification reaction is important in chemical biology and peptide/protein chemistry. To this end, several modifications to the indole ring of Trp using such as organic radical reaction [2] and sulfenylation with S-protected cysteine sulfoxides [3] have already been reported. We have recently developed Npys-OPh(pF), a stable surrogate for Npys-Cl [4,5] with a similar reactivity for modifying the thiol group of Cys and its solid supported form was used for a solid-phase disulfide ligation. Furthermore, we have now found that Npys-OPh(pF) acts as a new sulfenylation reagent for the indole ring of Trp by the activation with thioethers such as Met and diethylsulfide under acidic conditions. This reaction enabled a new selective chemical modification of Trp. The details of the sulfenylation reaction, including its plausible reaction mechanism, will be discussed in this presentation.