Multifunctional Carbon Fiber–Nanotube Frameworks for Safe, Recyclable, High‐Performance Lithium‐Ion Batteries

ABSTRACT This study introduces a multifunctional carbon fiber–carbon nanotube (CFCNT) architecture as a lightweight, thermally stable, and recyclable current collector for lithium‐ion batteries (LIBs). Compatible with both graphite anodes and LiFePO 4 cathodes, the CFCNT platform reduces collector mass to 4.4 mg/cm 2 —substantially lower than conventional copper (10.1 mg/cm 2 ) and aluminum (5.1 mg/cm 2 ) while enhancing electrical conductivity and interfacial stability. Full pouch cells employing CFCNT collectors achieve an initial capacity of 153 mAh/g and retain 126 mAh/g after 150 cycles (0.11% fade per cycle), with > 91% coulombic efficiency. Safety testing reveals minimal thermal response (< 2°C rise) during nail penetration, underscoring robust mechanical and electrochemical resilience. Critically, the architecture enables direct recovery and reuse of electrodes and current collectors, supporting a closed‐loop recycling strategy. These results position CFCNT collectors as a viable pathway toward safer, high‐performance, and circular energy storage technologies.