We demonstrate herein the use of a one-dimensional metal-organic material as a new type of electrode material for lithium-ion batteries (LIBs) in place of the classic porous three-dimensional materials, which are subject to the size of the channel for lithium-ion diffusion and blocking of the windows of the framework by organic solvents during the charging and discharging processes. Introducing a one-dimensional coordination compound can keep organic active substances insoluble in the electrolyte during the charging and discharging processes, providing a facile and general new system for further studies. The results show that both the aromatic ligand and the metal center can participate in lithium storage simultaneously, illustrating a new energy storage mechanism that has been well-characterized by X-ray photoelectron spectroscopy, electron paramagnetic resonance spectroscopy, and cyclic voltammetry. In addition, the fact that the one-dimensional chains are linked by weak hydrogen bonds rather than strong π-π stacking interactions or covalent bonds is beneficial for the release of capacity entirely without the negative effect of burying the active sites.