Both gold nanostructures and carbon nanotubes are rapidly emerging platforms for amperometric biosensor detection. Homogeneous display of biomolecular ligands is a key process in forming nanoscale array biosensors, improving the chances for sufficient signal strength and reproducibility at the limits of sensor geometries. The use of self-assembling interfaces on gold electrodes and CNT arrays enables homogeneous display, solvent access, target capture, sensor surface regeneration and potential for molecular wiring. Our approach uses an anchor peptide, covalently linked to the sensor surface, that is able to non-covalently capture probe labeled targets in solution with a high affinity and minimal surface leaching. The use of non-disrupting, metal-chelating scaffolds within the coiled coil sequence was tested for molecular wiring capabilities using model redox targets. Recombinant cassette production of probe sequences was investigated as a means to enable control over spatial and stoichiometric placement of redox active mediators and/or biomolecules. This thesis defines potential challenges as well as opportunities for future developments.

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