<p>The increasing severity of global water scarcity and atmospheric pollution has made the development of efficient and sustainable remediation materials a key research priority. High specific surface area, modulable pore architectures, and a large number of active sites make metal–organic frameworks (MOFs) highly promising for adsorption and catalytic processes. However, their applications are restricted by nanoparticle agglomeration, difficult recovery, and weak structures. Electrospinning offers an efficient strategy to alleviate these issues by embedding MOFs into polymeric nanofibers. The freestanding membranes exhibit three-dimensionally interconnected porous networks that enhance the MOFs dispersion, operation stability, and handling convenience. In this review, we summarize the design strategies, mechanistic understandings, and function performance of electrospun MOFs-based nanofibrous membranes in water purification (including pharmaceutical residues, heavy metal ions, synthetic dyes, and emulsified oils), and in air purification (including ultrafine particulate matter (PM) and volatile organic compounds (VOC)), compared with their counterparts. Moreover, we highlight recent advances in designing multifunctional synergistic systems, stimuli-responsive membranes, and materials with enhanced environmental resistance. Finally, emerging challenges and future research directions are discussed to provide insights for rationally designing advanced MOFs-integrated membrane technologies.</p>