Gold nanoparticles are metallic nanostructures with wide range of applications in biomedicine and biosensing. Among diverse morphologies of gold nanostructures, gold nanorods have attracted much more attention for their outstanding structure, optical property and function. The unique characteristic of these nanostructures encourages their integration with biomolecules of interest for versatile biomedical proposes. In this effort, amyloid fibrils with well-known mechanical strength and chemical stability have been used as biotemplates for assembly of gold nanorods to exploit dual property of both nano and bio counterparts in a hybrid nanoscaffold. To maximize the interaction of the nanostructures with the biotemplate, surface of the gold nanorods was modified with biocompatible polystyrene sulfonate (PSS). Spectroscopic and microscopic techniques including UV–Vis, CD, ThT and TEM were used to characterize formation of insulin amyloid fibrils, gold nanorods and their assemblies on the biotemplate. Morphology of gold nanorods was also monitored upon interaction with amyloid fibrils. Electrochemical impedance spectroscopy of the hybrid nanoscaffold showed that increase in the concentration of the assembled nanostructures on the biotemplate has clearly led to enhancement of conductivity. Results of this investigation highlight gold nanorods as promising candidates in design and fabrication of novel hybrid nanoscaffolds of enhanced conductivity, especially for biosensing and tissue engineering purposes.