An efficient NCS-promoted thiocyanation of pyrrolo[1,2-a]quinoxalines with NH4SCN or KSCN is described. A series of diverse 1-thiocyanatopyrrolo[1,2-a]quinoxalines were obtained in good yields with excellent functional group tolerance. With a similar strategy, the selenocyanation of pyrrolo[1,2-a]quinoxalines with KSeCN is also achieved. Importantly, this approach features mild reaction conditions, broad substrate scope, and gram-scale synthesis. Moreover, the transformations of the products are also further examined.