Captopril (CAP) is a safe, cost-effective, and environmentally organic compound that can be used as an effective organo-catalyst. Functional groups of captopril make it capable to attach to solid support and acting as promoters in organic transformations. In this work, captopril was attached to the surface of magnetic graphene nitride by employing a linker agent. The synthesized composite efficiently catalyzed two multicomponent reactions including the synthesis of 1,2,3,6-tetrahydropyrimidine and 2-amino-4H-chromene derivatives. A large library of functional targeted products was synthesized in mild reaction conditions. More importantly, this catalyst was stable and magnetically recycled and reused for at least five runs without losing catalytic activity.