The chemical composition and electrochemical properties of thin films polymerized from ferrocene and vinylferrocene under pulsed plasma conditions are reported. Relatively large scale and systematic variations in composition and properties of these films are observed with progressive changes in the pulsed duty cycles employed during synthesis, all other plasma variables being held constant. Compositional changes in both percent Fe content and the ratio of Fe-II/Fe-III with variations in the duty cycles are clearly shown by X-ray photoelectron spectroscopy analysis of these films. Voltammetric studies of the plasma-polymerized films deposited on glassy carbon electrodes provide additional evidence for the variations in the electroactive iron content of the films with changes in the pulsed plasma duty cycles employed during synthesis. Overall, the results of this study provide further support for the utility of the pulsed plasma technique to provide controlled film composition during synthesis of organometallic films.