Abstract: | An efficient three‐component reaction of aromatic aldehydes, 6‐aminouracil/6‐amino‐1,3‐dimethyluracil and 4‐hydroxycoumarin in the presence of a novel heterogeneous catalyst H3PMo12O40‐immobilized Co3O4/chitosan led to a synthesis of a new class of pyrimidinedione derivatives under reflux conditions. The magnetically recoverable nanocomposite of Co3O4/chitosan/H3PMo12O40 was fully characterized by Fourier transform‐infrared spectrophotometry, scanning electron microscopy, X‐ray powder diffraction, energy‐dispersive X‐ray spectroscopy, vibrating‐sample magnetometry and N2 adsorption–desorption by Brunauer–Emmett–Teller analysis. Results show that Keggin‐type 12‐molybdophosphoric acid immobilized into the network of the cross‐linked chitosan with super‐paramagnetic Co3O4 nanoparticles. The present method offers several advantages, such as simple procedure, short reaction times and excellent yields of products. The novelty of the catalyst, high catalytic activity, easy separation from the reaction with an external magnetic field and reusability of the catalyst in six consecutive runs are additional eco‐friendly attributes of this catalytic system. |