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Being closely associated with a variety of physiological and pathological processes, matrix metalloproteinases (MMPs) are useful as potential targets for drug therapy and informative markers for disease diagnosis. On the basis of the electrochemically induced grafting of ferrocenyl polymers and the proteolytic cleavage of recognition peptide, a novel electrochemical sensor is presented in this work for the highly specific interrogation of MMP activities at ultralow levels. The recognition peptide, to be immobilized via the N-terminus, i