Mechanically Unwinding Carbon Nanotubes Enables Homogeneous Conductive Networks in High‐Loading Dry Cathodes for Lithium‐Ion Batteries

The expanding electric vehicle market has driven an urgent demand for high‐energy‐density lithium‐ion batteries (LIBs). Solvent‐free dry‐processed electrodes offer strong potential for thick electrode development, but increasing thickness exacerbates the difficulty of uniformly dispersing conductive additives, posing a significant challenge for efficient electron and Li‐ion transport. Herein, we report mechanically pre‐unwound carbon nanotubes (uCNTs) as a morphologically engineered conductive additive with superior dispersibility, enabling continuous and homogeneous conductive networks in high‐loading Ni‐rich NCM811 cathodes. Ultra‐thick dry electrodes (10.5 mAh cm −2 , 170 μm) were realized using only 0.5 wt% uCNT—a threefold reduction compared with carbon black—yet delivered 120% higher capacity at 3.0 C and 92.7% capacity retention after 50 cycles. Furthermore, uCNT/natural graphite pouch full‐cells (5.0 mAh cm −2 , N/P ratio 1.1) demonstrated 89.5% capacity retention with an average Coulombic efficiency of 99.7% after 200 cycles at 0.2 C, validating the practical applicability of uCNT‐based dry electrodes. These results show that enhanced CNT dispersibility enables continuous conductive networks that alleviate the long‐standing ionic‐electronic transport imbalance in thick electrodes. This work provides a practically scalable, solvent‐free pre‐unwinding strategy that establishes a viable pathway for next‐generation high‐energy LIBs, coupling superior electrochemical performance with sustainable and industrially relevant manufacturing.