Carbon nanostructural materials have gained the spotlight as promising anode materials for energy storage; they exhibit unique physico-chemical properties such as large surface area, short Li + ion diffusion length, and high electrical conductivity, in addition to their long-term stability. However, carbon-nanostructured materials have issues with low areal and volumetric densities for the practical applications in electric vehicles, portable electronics, and power grid systems, which demand higher energy and power densities. One approach to overcoming these issues is to design and apply a three-dimensional (3D) electrode accommodating a larger loading amount of active anode materials while facilitating Li + ion diffusion. Furthermore, 3D nanocarbon frameworks can impart a conducting pathway and structural buffer to high-capacity non-carbon nanomaterials, which results in enhanced Li + ion storage capacity. In this paper, we review our recent progress on the design and fabrication of 3D carbon nanostructures, their performance in Li-ion batteries (LIBs), and their implementation into large-scale, lightweight, and flexible LIBs.