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Abstract The utilization of binders has severely hindered ionic diffusion and electron transfer in the traditional lithium‐ion battery. Herein, a self‐standing hard carbon film using nanocellulose as precursor has been constructed as binder‐free electrodes via two‐step thermal treatment. The cyclization and aromatization of small molecular fragments promote the formation of hyper‐crosslinked framework with abundant welded junctions. Importantly, carbon nanofibers not only serve as an inter‐connected conductive network for fast electron transfer, but also as an interlinked mechanical skeleton for convenient Li+ diffusion and electrode structural stability. Furthermore, the optimized carbon film, with accessible redox‐active carbonyl groups (CO) and abundant micropores, is beneficial for Li+ accommodation. It exhibits high reversible capacity of 513.1 mAh g−1 at 50 mA g−1 and excellent cycle stability to extend over 1000 cycles without signs of decay. This study provides an efficient strategy for the design of high‐performance biomass‐derived anode materials with stable‐structure for alkaline batteries.