Electrochemical energy storage is one of the important technologies for a sustainable future of our society, in times of energy crisis. Lithium-ion batteries and supercapacitors with their high energy or power densities, portability, and promising cycling life are the cores of future technologies. This Review describes some materials science aspects on nanocarbon-based materials for these applications. Nanostructuring (decreasing dimensions) and nanoarchitecturing (combining or assembling several nanometer-scale building blocks) are landmarks in the development of high-performance electrodes for with long cycle lifes and high safety. Numerous works reviewed herein have shown higher performances for such electrodes, but mostly give diverse values that show no converging tendency towards future development. The lack of knowledge about interface processes and defect dynamics of electrodes, as well as the missing cooperation between material scientists, electrochemists, and battery engineers, are reasons for the currently widespread trial-and-error strategy of experiments. A concerted action between all of these disciplines is a prerequisite for the future development of electrochemical energy storage devices.