Environmental pollution has emerged as a critical global concern due to the release of pollutants from industries, agricultural fields, and other human activities, requiring urgent attention and sustainable solutions. Metal–Organic Frameworks (MOFs) are porous materials consisting of organic ligands and inorganic metal ions or clusters. They have been introduced as a promising class of material for environmental remediation. Their variable pore size, large surface area, and diverse structural and functional properties make them suitable for environmental applications. Water purification through the removal of heavy metals, dyes, toxins, and organic pollutants have been achieved through these materials. The removal of harmful gases (carbon dioxide, sulphur dioxide, ammonia) from the environment is another important application of MOFs. This paper gives a critical insight into the mechanistic pathways of MOFs in adsorption, photocatalysis, redox-mediated degradation, and ion-exchange processes used for the removal of pollutants. The structural features of MOFs influence contaminant capture, selectivity, and degradation kinetics. Recent studies employing in situ spectroscopy, computational modeling, and kinetic analysis have unraveled the interaction dynamics between MOFs and pollutants. By bridging structural attributes with mechanistic functions, this paper will be helpful in the further exploration of MOFs, with potential to restore the environment.