Flexible supercapacitors (SCs) have attracted increasing attention as the power supply unit for portable/wearable electronics. Carbon nanotubes (CNTs) are promising candidate materials for flexible SC electrodes because of their outstanding mechanical property, high electrical conductivity, large surface area, and functionability. CNTs can assemble into various macroscopic materials with different dimensions. In this review, flexible CNT assemblies including 1D fibers, 2D films, and 3D aerogels and sponges are introduced with a focus on the design strategies and fabrication techniques. The recent developments and state-of-the-art applications of such structures as electrodes in flexible SCs are summarized based on device configurations including sandwiched, interdigital in-plane, and cable-type configurations. The flexible CNT-based electrodes have shown great advantages in bendability, stretchability and/or compressibility, as well as a long cycle lifetime. The current challenges and future research opportunities in this field are also discussed.

Flexible batteries, which maintain their functions potently under various mechanical deformations, attract increasing interest due to potential applications in emerging portable and wearable electronics. Significant efforts have been devoted to material synthesis and structural designs to realize the mechanical flexibility of various batteries. Carbon nanotubes (CNTs) have a unique one-dimensional (1D) nanostructure and are convenient to further assemble into diverse macroscopic structures, such as 1D fibers, 2D films and 3D sponges/aerogels. Due to their outstanding mechanical and electrical properties, CNTs and CNT-based hybrid materials are superior building blocks for different components in flexible batteries. This review summarizes recent progress on the application of CNTs in developing flexible batteries, from closed-system to open-system batteries, with a focus on different structural designs of CNT-based material systems and their roles in various batteries. We also provide perspectives on the challenges and future research directions for realizing practical applications of CNT-based flexible batteries.