Structural biomimicry is a fascinating concept to explore hierarchically organized nanomaterials for mechanical structures, catalysis, sensing, and energy storage applications. Here we report the fabrication of biomimetic mesoporous cobalt ferrite/carbon nanoflake materials with helical morphologies and evaluate their electrochemical properties as free‐standing lithium‐ion battery (LIB) anodes. Iridescent chiral nematic mesoporous chitosan films obtained from crab shells were combined with binary metallic ions to afford helical cobalt ferrite/chitosan membranes. The cobalt ferrite/chitosan composites were thermally converted to cobalt ferrite/carbon replicas with hybrid nanoflakes arranged in a twisted Bouligand‐type mesoporous network. The structure of the materials was probed by electron microscopy, powder X‐ray diffraction, and Raman spectroscopy. We directly used these freestanding cobalt ferrite/carbon films as binder‐ and additive‐free LIB anodes, where they showed a first discharge capacity of 862 mAh g−1 (at 100 mA g−1), which faded during subsequent charge‐discharge cycles. Our work demonstrates a new potential use of chiroptical chitosan membranes to develop energy storage materials, a process that may be extended to other metal‐oxide based components.