Metal-organic frameworks (MOFs) hold considerable promise for environmental remediation owing to their exceptional performance and distinctive structure. Nonetheless, the practical implementation of MOFs encounters persistent technical hurdles, notably susceptibility to loss, challenging recovery, and potential environmental toxicity arising from the fragility, insolubility, and poor processability of MOFs. MOF-based three-dimensional macrostructures (3DMs) inherit the advantageous attributes of the original MOFs, such as ultra-high specific surface area, tunable pore size, and customizable structure, while also incorporating the intriguing characteristics of bulk materials, including hierarchical structure, facile manipulation, and structural flexibility. Consequently, they exhibit rapid mass transfer and exceptional practicality, offering extensive potential applications in environmental remediation. This review presents a comprehensive overview of recent advancements in utilizing MOF-based 3DMs for environmental remediation, encompassing their fascinating characteristics, preparation strategies, and characterization methods, and highlighting their exceptional performance in pollutant adsorption, catalysis, and detection. Furthermore, existing challenges and prospects are presented to advance the utilization of MOF-based materials across various domains, particularly in environmental remediation.