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This review article comprehensively explores the electrochemical detection of organophosphate-based agents, including warfare agents, pesticides, and simulants. It provides an in-depth analysis of their molecular structures, emphasizing the inherent toxicity and environmental risks posed by these compounds. The review highlights the significant role of flexible sensors in facilitating the electrochemical detection of organophosphate-based agents, offering insights into their design, development, and application in detection methodologies. Additionally, the article critically evaluates the challenges encountered in this field, such as sensor sensitivity and sample complexity, and discusses potential solutions to address these challenges. Furthermore, it outlines the future scope and opportunities for advancement in electrochemical detection technologies, including the integration of novel materials and the exploration of innovative detection strategies. By synthesizing current research findings and identifying future research directions, this review contributes to the ongoing discourse on the detection and mitigation of organophosphate-based agents’ risks to human health and the environment.