The organometallic complexes (OMCs) are formed through the coordination between the metal nodes and the organic ligands. Due to the diversity of the organic ligands, the OMCs have various structures and thus may be adopted on a broad range of occasions. In this chapter, we focus on the OMCs adopted as electrode materials in the energy storage area. According to the structure of OMCs, we categorize them into small molecules, 1D, 2D, and 3D metal-organic frameworks (MOFs). In each part, the structures of the OMCs are briefly introduced, and the resultant functions and advantages of the OMC-based electrodes in the secondary batteries are discussed. Finally, a summary and an outlook about the OMC-based electrodes are supplied, with the aim to inspire more work in the more stable and high-energy OMC-based electrodes.