The introduction of hierarchy and chirality into structure is of great interest, and can result in new optical and electronic properties due to the synergistic effect of helical and anisotropic structures. Herein, we demonstrate a simple and straightforward route toward the fabrication of hierarchical chiral materials based on the assembly of two-dimensional graphene oxide nanosheets (GO) and one-dimensional cellulose nanocrystals (CNCs). The unique layered structure of CNC/GO could be preserved in the solid state, allowing electrode active SnO2 to be loaded for potential applications in energy storage. The resultant SnO2/CNC/reduced GO (SnO2/CNC/rGO) composite could be processed into film, fiber, and textile with an extremely high tensile strength of 100 MPa. The free-standing SnO2/CNC/rGO electrodes exhibit highly improved energy storage performance, with a reversible capacity of ∼500 mA h g-1 maintained for 1500 cycles in the film and ∼800 mA h g-1 maintained for 150 cycles in the textile at a current density of 500 mA g-1. This is attributed to the prepared hierarchical chiral structures. The presented technique provides an effective approach to producing hierarchical functional materials from nanoparticles as building blocks, which might open an avenue for the creation of new flexible energy storage devices.