New developments in laser ablation have shown great potential as nanofabrication methodologies, offering many significant advantages over more traditional methods. Herein, we have developed a method for applying two of these techniques, confined atmospheric pulsed-laser (CAP) deposition and laser ablation synthesis in solution (LASiS), to the fabrication of a nanostructured sensor platform. Following deposition, additional steps were then used to crosslink the deposited nanostructures and fabricate counter and reference electrodes. Chronoamperometry and cyclic voltammetry (CV) were used to assess the effects of these crosslinking steps on the properties of the sensor surfaces. These experiments resulted in the development of a simple, inexpensive and readily scalable process for the fabrication of 3-electrode sensor systems. As an example of a readily measurable surface interaction, electrochemical impedance spectroscopy (EIS) was applied to demonstrate the use of these systems in the detection of 6-mercaptohexanol. This interaction was examined in real-time by measuring the change in the EIS of the sensor system over time following its exposure to the thiol. This experiment clearly showed a measurable EIS response, demonstrating the effectiveness of these newly fabricated sensors for the detection of a simple surface interaction and suggesting the future potential of these laser based methods as the basis for an inexpensive, facile, rapid and scalable sensor fabrication process.