Although lithium-ion batteries and supercapacitors have shown rapid progress over the last two decades, next-generation energy storage applications, such as fast-evolving portable electronics, electrified propulsion, and load-leveling for renewable energy systems, require multi-functional energy sources that have both high-energy and -power, long cycle life, and flexibility, exceeding the performance of conventional energy storage devices. Aiming towards such advanced energy storage technologies, Dr. Lee’s research pays particular attention to harnessing charge storage reactions of nanostructured electrodes and their nano-fabrication processes. In this presentation, we will discuss our recent progress on designing multi-functional electrode materials.  We will first show that redox-active organic electrodes prepared from earth-abundant organic materials can be promising cathodes for large-scale energy storage devices. We reveal that these organic electrodes have promising charge storage properties for both Li- and Na-ion storage. The assembled organic electrodes are employed as cathodes for hybrid capacitors and Li- and Na-ion batteries, delivering high capacity with superior power capability and cycling stability. Thus, these high-performance organic electrodes can be promising cathodes for large-scale rechargeable batteries or hybrid capacitors. Next, we will introduce a new self-assembly technique, called a ligand-exchange induced layer-by-layer assembly, which can fine-tune the interface structures of the assembled nanoparticles. Based on this technique, we systematically assemble the 3D nanostructured electrodes consisting of conductive and charge storage nanoparticles with controlled distance, composition, and alignment. We control the interface structures and corresponding charge transfer and storage properties of the assembled 3D nanostructured electrodes, demonstrating flexible and wearable energy storage and conversion devices.