Abstract <p>A novel and environmentally benign electrochemical method has been developed for the regioselective C6 thiocyanation of tetrahydroquinolines using potassium thiocyanate (KSCN) as an inexpensive and readily available thiocyano source. This transition-metal-free and oxidant-free protocol proceeds under mild conditions, enabling efficient construction of C(sp²)-SCN bonds. Utilizing TEMPO as a redox mediator, the reaction affords 6-thiocyanato-tetrahydroquinoline derivatives in moderate to good yields. The protocol is also applicable to the C4 thiocyanation of anilines and the C6 selenocyanation of tetrahydroquinolines. The method demonstrates excellent regioselectivity, high atom economy, broad substrate scope, and good functional group compatibility, providing a practical approach to a range of valuable thiocyanated and selenocyanated derivatives.</p> Graphical Abstract <p>An environmentally benign electro-chemical method for the regioselective C6 thio-/selenocyantion of tetrahydroquinolines.</p> <p></p>