Simple solid-state mixing and calcination of catalytic amounts of metal-organic frameworks (MOFs) in the presence of aluminosilicates allow for the generation of active and robust supported metal oxide nanoparticles that catalyze C–C and C–N bond formations. The proposed Cu and Zn containing aluminosilicates outperform state-of-the-art solid catalysts for the synthesis of various aza-heterocycles under mild and heterogeneous conditions, exhibiting the highest turnover frequencies (TOFs) ever reported for cost-efficient and reusable CuO and ZnO active sites.