Addressing the global challenges of water scarcity and pollution requires the development of advanced water treatment technologies that are both environmentally compatible and economically viable. Traditional water treatment methods often suffer from high energy consumption and the risk of secondary pollution. In contrast, membrane separation technology, with its low energy consumption, high efficiency, ease of operation, and lack of secondary pollution, has gained a prominent position in the water treatment field. Particularly, graphene oxide membranes (GOm) have shown great potential due to their unique two-dimensional nanostructure and tunable physical and chemical properties. Despite the impressive performance of GOm, precise microstructural control remains a significant challenge, directly affecting the membrane’s separation efficiency and selectivity. This paper thoroughly explores the key parameters influencing GOm performance, including channel size, water stability, degree of oxidation, charge density, and wettability. Notably, this review focuses on the research progress in using metal–organic frameworks (MOF) for the micro-tuning of GOm. The highly ordered porous structure of MOF provides new avenues for regulating GOm, enhancing their separation performance and paving the way for the development of novel, efficient water treatment membrane materials. The review comprehensively analyzes the latest research findings on MOF-GOm composites, offering in-depth insights and strategies aimed at driving innovation and application in water treatment technologies. It provides scientific foundations and technical support for the sustainable utilization of global water resources.