Topological Structure‐Modulated Collagen Carbon as Two‐in‐One Energy Storage Configuration toward Ultrahigh Power and Energy Density

Efficient energy storage devices with suitable electrode materials, that integrate high power and high energy, are the crucial requisites of the renewable power source, which have unwrapped new possibilities in the sustainable development of energy and the environment. Herein, a facile collagen microstructure modulation strategy is proposed to construct a nitrogen/oxygen dual‐doped hierarchically porous carbon fiber with ultrahigh specific surface area (2788 m 2 g −1 ) and large pore volume (4.56 cm 3 g −1 ) via local microfibrous breakage/disassembly of natural structured proteins. Combining operando spectroscopy and density functional theory unveil that the dual‐heteroatom doping could effectively regulate the electronic structure of carbon atom framework with enhanced electric conductivity and electronegativity as well as decreased diffusion resistance in favor of rapid pseudocapacitive‐dominated Li + ‐storage (353 mAh g −1 at 10 A g −1 ). Theoretical calculations reveal that the tailored micro−/mesoporous structures favor the rapid charge transfer and ion storage, synergistically realizing high capacity and superior rate performance for NPCF‐H cathode (75.0 mAh g −1 at 30 A g −1 ). The assembled device with NPCF‐H as both anode and cathode achieves extremely high energy density (200 Wh kg −1 ) with maximum power density (42 600 W kg −1 ) and ultralong lifespan (80% capacity retention over 10 000 cycles).