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Nitrogen-incorporated tetrahedral amorphous carbon (ta-C:N) has electrochemical properties that are comparable to boron-doped diamond (BDD), but can be deposited at low temperatures, and is scalable across substrate areas substantially exceeding what is currently possible for BDD. Most published studies of ta-C:N electrodes focus on films deposited on conductive substrates due to the relatively high resistivity of ta-C:N compared to other carbon and metal-based electrodes. However, some of the most compelling applications of electrochemistry, for example, optically transparent spectroelectrochemical devices, require insulating substrates such as fused silica glass (FSG) or polymers. In this study, we deposited 50 nm of ta-C:N by laser controlled pulsed cathodic vacuum arc (Laser-Arc) onto insulating FSG to investigate the electrochemical response compared to conductive silicon (c-Si) substrates. No oxidation or reduction of potassium ferrocyanide during cyclic voltammetry (CV) could be observed at the FSG electrode. To address this, we introduced a 5 nm chromium (Cr) interlayer deposited by magnetron sputtering between ta-C:N and FSG. This electrode configuration led to clear cathodic and anodic CV peaks of potassium ferro/ferricyanide but with an increased peak separation compared to the c-Si electrode. However, the peak separation could be reduced to values comparable to ta-C:N deposited on c-Si by optimizing Cr sputtering conditions and introducing an argon plasma pretreatment of the FSG surface. Atomic force microscopy revealed that these changes improved the Cr growth homogeneity, which in turn increased the electrical conductivity of the Cr interlayer as determined by 4-point probe measurements. [ABSTRACT FROM AUTHOR]