Metal-organic frameworks (MOFs) attract significant attention due to their favorable surface characteristics and high adsorption potential; however, their application is mainly limited by poor stability and unsuitable pore sizes. The development of MOF-based composites has shown improved performance over their pristine counterparts, yet systematic classification and detailed insights into their binding abilities with different materials for specific pollutants remain underexplored. Additionally, a comparative analysis of the advanced properties of MOF-based composites versus pristine MOFs is lacking. This review aims to provide a detailed comparison, highlighting the limitations of pristine MOFs and the notable improvements achieved through composite formation, particularly regarding structural stability, material properties, adsorptivity, and reusability for removing organic pollutants. The synthesis methods are critically evaluated, emphasizing the need for greener and more sustainable fabrication routes. Mechanistic aspects of adsorption processes, along with regeneration performance and experimental parameters, are discussed to offer a comprehensive perspective. Furthermore, the review addresses key challenges such as toxicity concerns, industrial applicability, and cost-effectiveness, which hinder large-scale use of MOF-based technologies in wastewater treatment. Future strategies are proposed to guide research toward developing cost-effective, eco-efficient, and scalable MOF composites aligned with the Sustainable Development Goals.