In this study, new magnetic reduced graphene oxide aerogel/HKUST-1 nanocomposite was designed and synthesized given the transformation of graphene oxide sheets to three-dimensional reduced graphene oxide aerogel, the in-situ magnetization of aerogel substrate, and the in-situ formation of HKUST-1 particles. Apart from characterizing the chemistry and structure of the designed magnetic nanocomposite (FT-IR, EDX, ICP, FE-SEM, DLS, XRD, VSM, and TG analyses), its catalytic performance was evaluated in the one-pot synthesis of biologically active 1,8-dioxo-decahydroacridine and polyhydroquinoline derivatives. The combination of magnetized reduced graphene oxide aerogel and HKUST-1 in the form of a new heterogeneous magnetic nanocatalyst was accompanied by a high synergetic catalytic effect in the symmetric and unsymmetrical Hantzsch condensation reactions. Compared to previous research studies, the pharmaceutical 1,8-dioxo-decahydroacridine and polyhydroquinoline derivatives can be synthesized using a partial amount of this nanocatalyst with a high percentage of yields in a short reaction time.