Macromolecules containing metals combine the processing advantages of polymers with the functionality offered by the metal centers. This review outlines the progress and recent developments in the area of electrochemical chemo/biosensors that are based on organometallic polymers. We focus on materials in which the metal centers provide function, allowing these materials to be used in electrochemical sensing applications based on various transduction mechanisms. Examples of chemo/biosensors featuring organometallic polymers that possess Fe, Os, Co and Ru are discussed.