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In this publication, we reported an efficient one-pot, four-component procedure for the synthesis of 2,6-diamino-4-Aryl-4H-Thiopyran-3,5-dicarbonitrile derivatives by a reaction between primary amines, carbon disulfide, malononitrile, and benzylidenemalononitrile in the presence of magnetic NH2.MIL-101(Fe)/ED as a basic metal organic framework catalyst. Magnetic NH2.MIL-101(Fe)/ED was synthesized through anchoring FeCl3 on CoFe2O4 magnetic nanoparticles surface and then 2-aminoterphthalic acid was used to form MOF structure. At the final step, metal centers were modified with ethylenediamine (ED). The different techniques such as Fourier transmission infrared spectroscopy, X-ray diffraction, Field emission scanning electron microscopy, Transmission electron microscopy, Brunauer-Emmett-Teller analysis, and Thermogravimetric analysis were used to characterize the structure of the catalyst. Using X-ray crystallography, the structure of the final product was also determined.