Herein, we synthesized biological magnetic glycoluril tetrakis(methylene phosphorous acid) as a new heterogeneous nano-catalyst. The magnetic nano-catalyst Fe3O4@GTMPA was used for the synthesis of diphenyl nicotinonitrile derivatives by multi-component reaction of wide spread aldehydes, acetophenones, ammonium acetate, and 3-(1H-indol-3-yl)-3-oxopropanenitrile in the solvent-free conditions at 110 C. The final step of reaction mechanism was preceded via a cooperative vinylogous anomericbased oxidation (CVABO) as green and convenient approach.