Herein, we describe the formation of silica structures on indium, tin oxide (ITO) surfaces using poly-L-lysine (PLL) to template the condensation of silicic acid. Precisely controlled electrostatic fields were used to preposition PLL onto ITO surfaces. Subsequent polypeptide-mediated silicification resulted in the formation of silica with concentration gradients that followed the pattern of the externally applied electrostatic field used in the deposition of the PLL. The resulting silica structures were securely attached to the ITO surface. The technique described here offers an inexpensive and rapid method for the deposition of polypeptides on surfaces.