In this paper we report the use of ferrocenyl-tethered dendrimer (Fc-D) as an electrode modifier supported by a self-assembled monolayer coated gold surface. The pretreatment of electrodes with Fc-D allows the covalent immobilization of glucose oxidase. The resulting integrated hybrid system provides electrical contact between the redox center of the enzyme and the electrode, and improves the overall bioelectrocatalyzed oxidation of glucose. Cyclic voltammetry combined with surface plasmon resonance (SPR) is used to investigate the redox-induced orientation changes of ferrocene-tethered dendrimers and the optimal electrical wiring of the enzyme, depending on the length of the alkyl chain of the ferrocene-tethered groups. The amount of substrate controls the steady-state concentration ratio of Fc/Fc(+) in the film composition. Therefore, the SPR spectrum of the film is controlled by the reversible change in the refractive index of the enzyme-integrated redox film. The proposed method demonstrates a new procedure for developing a stable amperometric redox enzyme-based sensor by designing a new nanostructured material that control the biosensing performance.