An iron-catalyzed cascade reaction of C(sp3)-Se bond cross-coupling/C-N bond formation was developed. Various 5,13a-dihydro-6H,8H-benzo[5,6][1,3]selenazino[2,3-a]isoquinolin-8-one derivatives were synthesized under mild conditions starting from 1,2,3,4-tetrahydroisoquinolines and 2-hydroselenobenzoic acids. This protocol provides an economical approach for C(sp3)-Se bond formation.