2D Tetrathiafulvalene‐Based Metal–Organic Framework Linked by Hydrogen Bonding for Boosting Long‐Cycle Stability of Lithium‐Ion Batteries

2D metal–organic frameworks (2D MOFs) represent an emerging class of materials distinct from conventional 3D MOFs (3D MOFs). In comparison to 3D MOFs, 2D MOFs exhibit unique characteristics such as ultrathin layers, high surface area, and accessible active sites, making them highly promising as functional materials. However, their practical application in electrochemical energy storage is hindered by poor electrical conductivity and stability. In this study, a 2D TTF‐Co‐MOF via hydrogen bonding is successfully synthesized, using a coordination polymerization method involving m‐H 4 ‐TTFTB ligand, DMF, H 2 O, and Co 2+ ions. This 2D MOF demonstrates excellent long‐term stability as an anode material for lithium‐ion batteries (LIBs). Remarkably, the corresponding LIB retains a nearly unchanged capacity even after thousands of charge–discharge cycles.