Chemical warfare agents (CWAs) pose a severe threat to both civilians and military personnel due to their extreme toxicity. The urgent necessity of creating a portable device for rapid on-site quantification of CWAs is evident. This article presents the design and synthesis of a specialized material, calix[4]pyrrole R2 modified zinc oxide nanohybrid material (R2-ZnO), and its utilization in crafting a smart portable electrochemical device (SPED). The detection capability of the R2-ZnO nanohybrid material was evaluated using various electrochemical techniques, specifically targeting the identification of CWAs' mimic compound, diethyl chlorophosphate (DCP). Upon interaction with the R2-ZnO nanohybrid material, DCP gets entrapped within the pyrrolic cavity of the R2-ZnO nanohybrid material and transforms into hydrolyzed, nontoxic compounds, resulting in a significant increase in current intensity. The interaction of DCP with the R2-ZnO nanohybrid material generates a quick response by enhancing the remarkable current density of the material. Surprisingly, when the R2-ZnO nanohybrid material was exposed to other organophosphates, there was no observable change in the current. Additionally, the developed SPED was tailored for the quantification of DCP, demonstrating fast response times within seconds of exposure. This pioneering research offers a promising pathway to develop a cost-effective, portable device for the rapid on-site quantification of hazardous CWAs.