A nanocomposite comprised of MoS₂-RGO having unique structural features was developed by using a facile preparation strategy and demonstrated to be a highly efficient heterogeneous catalyst for the synthesis of indole alkaloids in water. The catalyst could be recycled six times without signiï¬�cant loss of its activity. Green chemistry matrix calculations for the reaction showed high atom economy (A.E. = 94.7%) and small E-factor (0.089). Using this nanocomposite as catalyst, four naturally occurring indole alkaloids, Arundine, Vibrindole A, Turbomycin B, and Trisindole, were synthesized along with their other derivatives in excellent yields.