Abstract: Glassy metal-organic frameworks (MOFs) integrate the intrinsic characteristics of crystalline MOF, including abundant pore structures, tunable chemical compositions, and adjustable coordination environments, with the inherent advantages of glassy materials, such as long-range disorder, grain-boundary-free structures, and isotropic properties, demonstrating great potential in energy-related applications. In recent years, owing to their thermoplastic flowability, excellent film-forming capability, mechanical stability, and efficient ion transport properties, glassy MOF have attracted increasing attention for regulating the surface and interface properties of electrode materials. Glassy MOFs can form uniform and dense micro/nanoscale coating layers on the surfaces of both anode and cathode materials, effectively alleviating volume variations during charge/discharge processes. Meanwhile, their continuous disordered networks facilitate homogeneous ion transport, suppress dendrite growth on fast-charging electrodes such as graphite and alkali-metal anodes, and stabilize electrode interfaces. Furthermore, glassy MOFs-based interfacial layers can mitigate stress accumulation and structural degradation of cathode particles, inhibit transition-metal dissolution, stabilize electrode/electrolyte interfaces, and improve interfacial reaction kinetics, thereby enhancing the rate capability and cycling stability of electrodes. This review provides a comprehensive overview of recent advances in the application of glassy MOFs as surface and interfacial modification layers for electrode materials. The fundamental structural characteristics of glassy MOFs are first introduced, followed by a systematic discussion of their construction and performance regulation in the interfacial modification of graphite, silicon, phosphorus, lithium-metal anodes, and cathode materials. Particular emphasis is placed on elucidating their roles in mitigating volume expansion, suppressing dendrite growth, stabilizing interfacial structures, promoting ion transport, and optimizing interfacial kinetics. Finally, the current challenges and future perspectives of glassy MOFs-based materials are discussed, providing insights into their further development and application in advanced rechargeable battery systems.