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Cu(II)-modified nitrogen-rich covalent organic polymer (Cu/N-COP-1) was fabricated and employed to catalyze the cross-dehydrogenative ortho-aminomethylation of phenols. The Cu/N-COP-1 catalyst displayed excellent catalytic activity under mild conditions without any ligand. Various substituted phenols and N,N-dimethylanilines were successfully converted to the corresponding products. Moreover, the catalyst can be readily reused for at least five consecutive runs without obvious loss of catalytic activity. This can be attributed to the interaction between the nitrogen-containing group of the covalent organic polymer and Cu species, which makes Cu species steadily immobilized on the surface of polymer.