Metal cations, when present in appropriate concentrations, serve an essential physiological function, however, their presence in larger concentrations has proven to be detrimental to human health. Modern industrial processes such as alloy treatment, coatings, and leather pigmentation, often result in the release of the heavy metal cations, causing adverse biological and ecological consequences. Amongst many, hexavalent chromium (Cr6+) is a major concern because of its carcinogenic properties. Therefore, it is imperative to develop a sophisticated technique for the early detection of Cr present in aqueous solutions. Numerous methods use techniques such as mechanical, optical, spectroscopic, and electrochemical for the detection of contaminants in aqueous solutions. Electrochemistry driven sensors have shown promise due to their possibility of miniaturization and low-cost. However, early and trace detection of such contaminants remains a challenge. Recently, atomically thin allotropes of carbon such as graphene or graphene oxide have been used to fabricate ultra-responsive and selective sensor platforms, owing to its excellent electrical conductivity, high surface area for functionalization, and physicochemical stability. In this work, we examine the use of electrically conducting polymer and atomically thin carbon materials as electrodes for the development of electrochemical sensors. Nanocomposite electrode films have been synthesized, and its performance as a function of number of cycles of deposition were analyzed. A capacitive microcomb sensor device has been fabricated, and the device performance using electrochemical, chemical, and morphological tests on electrodes as a function of deposition and electrolyte solutions will be highlighted. A fundamental understanding of reaction kinetics and identification of the rate-limiting steps will lead a path forward for developing robust sensors.