The grand challenge of a sustainable production and use of energy has focused research on the nanostructure of materials. This aspect is considered of critical importance for improving the performance of advanced materials and electrodes to meet demanding expectations. Carbon nanotubes (CNTs) are the first and most-successful example of nanomaterials, and play a central role in the development of advanced solutions for sustainable energy applications. However, notwithstanding the rising scientific and technological interest in CNTs, their use is still largely based on phenomenological observations that miss the complexities of the nanostructure and characteristics of these materials. This Concept paper addresses the need for a rational design of CNTs for energy applications, based on an understanding of the key aspects to be considered for their optimization in different applications such as lithium ion batteries, supercapacitors, solar cells, and fuel cells.