The present work describes the grafting of polymer-metal chelates (PMC) from Fe3O4@SBA-15 via the Surface Initiated-Atom Transfer Radical Polymerization (SI-ATRP) method. Fe3O4@SBA-15 were silylated by 2-bromo-2-methyl-N-(3-(trimethoxysilyl)propanamide (BTPAm) to give the surface-anchored ATRP initiator. Acrylamide (AAm) was polymerized from the Fe3O4@SBA-15 surface via the ATRP approach and trans-amidated with ethylenediamine to give poly(N-2-aminoethylacrylamide) grafted magnetic mesoporous silica, Fe3O4@SBA-g-PAE-AAm. The grafted chelating polymer ligand (CPL) was treated with an acetonitrile solution of Cu(OAc)2 to afford the Fe3O4@SBA-g-PAE-AAm-Cu(II). The grafted PMC was characterized by FT-IR, CP/MAS 13C NMR, thermo-gravimetric analysis (TGA), and Brunauer-Emmett-Teller (BET) analysis. The oxidation state of copper (+2) was confirmed using X-ray photoelectron spectroscopy (XPS). The catalytic activity of the grafted PMC was examined in the CO bond formation via the Ullmann-type O-arylation reaction between haloarenes and phenols after establishing the optimal reaction conditions. The excellent recyclability of the catalyst was shown by small deactivation over seven runs.