AbstractConducting polymers have been considered for use as cathode materials in rechargeable lithium‐ion batteries (LIBs) since 1981 but problems with poor cycling stability, rapid self‐discharge, and low energy and power densities have so far limited their applicability. Herein it is shown that nanostructured freestanding conducting polymer composites [e.g., polypyrrole (PPy) and polyaniline (PANI)] can be used to circumvent these shortcomings. Freestanding and binder‐free PPy and cellulose‐based composites can straightforwardly be used as versatile organic cathode materials for LIBs. The composite, reinforced with chopped carbon filaments (CCFs), exhibited a large active mass loading of approximately 10 mg cm−2, an areal capacity of 1.0 mAh cm−2(corresponding to 102 mAh g−1), and stable cycling. With an active mass loading of 4.4 mg cm−2, a capacity of 0.22 mAh cm−2(corresponding to 58 mAh g−1) was found for current densities of 5 A g−1yielding discharge times of approximately 40 seconds, and a capacity retention of 91 % over 100 cycles was obtained at 0.2 A g−1. The present method constitutes a straightforward approach for the manufacturing of high‐performance freestanding electroactive conducting‐polymer‐based paper‐like electrodes for use in inexpensive and sustainable, high‐performance organic LIBs.