This work minimizes the passive components of electrodes and moves toward bridging the gap between actual and theoretical battery gravimetric energy density. Binder‐free self‐supporting (BFSS) cathodes were prepared from redox‐active, high aspect ratio, potassium α‐MnO2 nanofibers (K‐OMS‐2) by eliminating the binder and current collector. The electroactive and structural element, K‐OMS‐2, was prepared by using a scalable, moderate temperature, aqueous synthesis. The BFFS electrode approach allows fabrication of thick, high energy density electrodes with low impedance, with up to 10‐fold improvement in delivered specific energy relative to conventional cathodes. This could enable the design of high‐capacity large form factor cells, as required for applications demanding high energy content. In principle, this approach suggests a widely applicable paradigm for the construction of other BFFS electrodes through the targeted synthesis of other transition‐metal oxides with high aspect, fibrous morphologies.