Direct attack of the bis(μ-oxo)dicopper core on an arene appears feasible in tyrosinase and model complexes on the basis of studies of new [Cu(III)/2(μ-O)2]2+ compounds supported by bidentate imine/amine ligands. In the first demonstration of such reactivity for a bis(μ- uxo)dicopper core, decomposition of these intermediates caused hydroxylation of a pendant phenyl ring [Eq. (a) in a reaction analogous to that catalyzed by tyrosinase.