Over recent decades, the widespread use of pesticides has been instrumental in securing a global food supply. However, this has led to significant environmental pollution concerns. Given the prevalent use of organophosphorus pesticides (OPs), there is an urgent need to develop sensors that can detect OPs with high selectivity and sensitivity. Electrochemical sensors offer an affordable and highly efficient solution for this challenge. Particularly, there have been remarkable advancements in creating metal–organic framework (MOF)-based electrochemical sensors. This review delves into the current advancements of MOF-based electrochemical sensors, emphasizing their use in detecting OPs. We investigate prevalent MOF modifications, detail methods for affixing MOF materials to various electrodes, and compare the electrochemical performance and stability of these methods. We also provide insights into the design principles of MOFs used in the electrochemical detection of OPs, breaking down the core detection mechanism. We hope our insights will guide researchers in developing sustainable, effective, and robust MOF-based portable electrochemical sensors.