In this paper, it is reported that the histidine-silane derivative Boc-His(Boc)-CONH-(CH2)3Si(OEt)3 can be polymerized via the sol-gel method or can be grafted on a silica surface. The obtained organosilicas bear histidine molecules covalently bonded on the inorganic matrix. Their Cu(II) complexes have been evaluated as oxidation catalysts for the conversion of 3,5-di-tert-butylcatechol (DTBC) to 3,5-di-tert-butylquinone (DTBQ) in the presence of dioxygen.