The MoS2-based reduced graphene oxide aerogel (MoS2-rGOA)-assisted organic transformation reactions are presented. MoS2-rGOA is used as a heterogeneous catalyst for the reduction of benzene derivatives such as benzaldehyde, nitrobenzene, and benzonitrile to benzyl alcohol, aniline, and benzamide and their derivatives, respectively, in green solvents (water/methanol) and green reducing agents (hydrazine hydrate having N2 and H2 as byproducts). The mechanistic features of the reduction pathway, substrate scope, and the best suitable conditions by varying the temperature, solvent, reducing agent, catalyst loading, time, etc. are optimized. All of the synthesized products are obtained in quantitative yield with purity and well characterized based on nuclear magnetic resonance analysis. Further, it is also observed that our catalyst is efficiently recyclable and works well checked up to 5 cycles.