Silica-precipitating polypeptides were deposited onto an indium tin oxide (ITO) surface from bulk solution with and without the assistance of an externally applied electrostatic field. Exposure of the peptide-coated surface to an alkoxide precursor produced biosilica structures that were securely attached to the electrode surface. The silica morphologies resulting from the test cases using an externally applied electrostatic field during peptide deposition were distinct from the morphologies resulting from cases without an applied field. The silica morphologies observed on the ITO surface were different from the usual silica morphology resulting from static conditions. Peptide size was also shown to influence resulting biosilica morphology. The experimental results presented herein demonstrate the feasibility of creating biosilica nanostructures with controlled morphologies using polypeptides in vitro.