Carbon nanotube-based materials are gaining considerable attention as novel materials for renewable energy conversion and storage. The novel optoelectronic properties of CNTs (e.g., exceptionally high surface area, thermal conductivity, electron mobility, and mechanical strength) can be advantageous for applications toward energy conversion and storage. Although many nanomaterials are well known for the unique structure-property relations, such relations have been sought most intensively from CNTs due to their extreme diversity and richness in structures. For the development of energy-related devices (like photovoltaic cells, supercapacitors, and lithium ion batteries), it is critical to conduct pre-evaluation of their design, operation, and performance in terms of cost, life time, performance, and environmental impact. This critical review was organized to address the recent developments in the use of CNT-based materials as working/counter electrodes and electrolytes in photovoltaic devices and as building blocks in next-generation flexible energy storage devices. The most promising research in the applications of CNTs toward energy conversion and storage is highlighted based on both computational and experimental studies along with the challenges for developing breakthrough products. (C) 2017 Elsevier Ltd. All rights reserved.