Microplastic (MPs) pollution has emerged as a worldwide environmental issue due to its constant presence in various ecosystems and potential threats to human health and biodiversity. In response to this concern, novel approaches are sought for effective microplastic removal. Metal–organic frameworks (MOFs), characterized by their high surface area, tunable porosity, and structural diversity, have gathered significant attention in recent years for their potential application in environmental remediation. This chapter delves into the fascinating field of MOFs and their unique properties that make them suitable for the removal of MPs from diverse environmental matrices. In subsequent sections, a detailed analysis of recent advancements in MOF synthesis methods and design strategies tailored for MP removal is presented. Furthermore, the drawbacks and challenges related to MOF stability, regeneration, and recyclability have also been highlighted and the avenues for further research in the field have been outlined. This chapter promises to deliver a comprehensive review of MOFs and their transformative potential in addressing the challenge of microplastic pollution while also providing insights into future research endeavors aimed at developing sustainable solutions to combat MP pollution.