Abstract The present lithium‐ion battery technology competition almost focuses on finding new materials, while less effort is invested in electrode engineering improvement with low‐cost. This study proposes a simple method of modulating the preferred orientation of crystal phases in LiCoO 2 electrode using a ≈500 mT magnetic‐field, cheaply and efficiently improving the performance of LiCoO 2 ||graphite pouch full batteries, including cycling stability, rate performance, and thermal safety performance. Under 3.0 C and 45 °C strict test conditions, LiCoO 2 ‐M ⊥ ||graphite battery even outputs the capacity retention rate of 42.8% after 1000 cycles, while that of pure‐LiCoO 2 battery is only 4.4%. Especially, the thermal runaway temperature of the battery needling experiment decreases by considerable 7.7 °C after magnetic‐field modulation. Comprehensive characterizations reveal that vertical magnetic field causes spin alignment of LiCoO 2 crystals along the (003) direction. This arrangement effectively improves the Li + diffusion dynamic and the interface compatibility of the electrode, suppressing the electrode polarization. During the cycling processes, the preferred orientation of LiCoO 2 particles forms an enhanced conductive network due to the formation of cross‐linked “Li + poor regions” on the surface, ultimately achieving significant performance improvement. This work can provide a potential low‐cost strategy for the production of commercial lithium‐ion batteries.