In this article, the synthesis of a novel and highly efficient recyclable and reusable heterogeneous nanocatalyst has been reported via the functionalizing of the Fe3O4‐magnetized graphene oxide nanosheets with the N6‐Schiff base Cu (II) complex (GO/Fe3O4@SPNC). The structure of this novel nanocatalyst was determined by different analytical techniques such as FTIR, FE‐SEM, TEM, TGA‐DTG, and VSM. The catalytic activity of the synthesized GO/Fe3O4@SPNC nanocatalyst was explored for the synthesis of several new 2H‐pyrido[3′,2′:6,7]pyrano[2,3‐d]pyrimidine‐7‐carbonitrile derivatives with excellent yields. All new derivatives were fully identified by various spectral (1H NMR, 13C NMR, FT‐IR, ESI‐MS) analyses. In addition, this nanocatalyst carried out satisfactory catalytic maintenance of activity and high chemical stability in the titled reactions after seven‐time of recycling without substantial loss of leaching.