A dioxomolybdenum(VI) complex of a Schiff base, immobilized on the surface of modified Fe3O4 with a silica coating, has been synthesized and characterized by spectroscopic and microscopic techniques including FTIR, TGA, ICP, SEM, EDX, VSM, and XRD analyses. The catalytic performance of this material has been evaluated for the preparation of 2-amino-4Hbenzo[ h]chromenes via the one-pot, three-component reaction of aldehydes, malononitrile, and 1-naphthol under solventfree conditions. The benefits of this protocol are short reaction time, simple workup procedure, and high yields of products. Also, the synthesized nanocatalyst could be separated easily from the reaction mixture using an external magnet and reused for four consecutive times with only minor degradation of its catalytic performance.