Compared to monometallic nanoparticles, bimetallic nanoparticles have attracted wide attention due to their physical properties, excellent catalytic activity, high regioselectivity, selectivity, and stability. Here, we have first synthesized 10 different kinds of graphene quantum dot–stabilized Cu-based bimetallic nanoparticles (including CoCu, NiCu, RuCu, RhCu, PdCu, AgCu, IrCu, AuCu, FeCu, and PtCu) and compared their catalytic activities in a CuAAC click reaction. Among them, RhCu provides the highest yield of the desired product in the click reaction (77%). The catalytic activity of these MCu in the click reaction is in the order: RhCu > PdCu > AuCu > CoCu > PtCu > AgCu > NiCu > CuNP > RuCu > FeCu > IrCu.