Metal-organic frameworks (MOFs) have recently emerged as ideal electrode materials and precursors for electrochemical energy storage and conversion (EESC) owing to their large specific surface areas, highly tunable porosities, abundant active sites, and diversified choices of metal nodes and organic linkers. Both MOF-based and MOF-derived materials in powder form have been widely investigated in relation to their synthesis methods, structure and morphology controls, and performance advantages in targeted applications. However, to engage them for energy applications, both binders and additives would be required to form postprocessed electrodes, fundamentally eliminating some of the active sites and thus degrading the superior effects of the MOF-based/derived materials. The advancement of freestanding electrodes provides a new promising platform for MOF-based/derived materials in EESC thanks to their apparent merits, including fast electron/charge transmission and seamless contact between active materials and current collectors. Benefiting from the synergistic effect of freestanding structures and MOF-based/derived materials, outstanding electrochemical performance in EESC can be achieved, stimulating the increasing enthusiasm in recent years. This review provides a timely and comprehensive overview on the structural features and fabrication techniques of freestanding MOF-based/derived electrodes. Then, the latest advances in freestanding MOF-based/derived electrodes are summarized from electrochemical energy storage devices to electrocatalysis. Finally, insights into the currently faced challenges and further perspectives on these feasible solutions of freestanding MOF-based/derived electrodes for EESC are discussed, aiming at providing a new set of guidance to promote their further development in scale-up production and commercial applications.

Assembling titanium carbide (Ti ₃ C ₂ T _x ) MXene nanosheets into macroscopic films presents challenges, including voids, low orientation degree, and weak interfacial interactions, which reduce mechanical performance. We demonstrate an ultrastrong macroscopic MXene film using liquid metal (LM) and bacterial cellulose (BC) to sequentially bridge MXene nanosheets (an LBM film), achieving a tensile strength of 908.4 megapascals. A layer-by-layer approach using repeated cycles of blade coating improves the orientation degree to 0.935 in the LBM film, while a LM with good deformability reduces voids into porosity of 5.4%. The interfacial interactions are enhanced by the hydrogen bonding from BC and the coordination bonding with LM, which improves the stress-transfer efficiency. Sequential bridging provides an avenue for assembling other two-dimensional nanosheets into high-performance materials.