LiFePO₄emerges as a viable alternative to cobalt‐containing cathodes, such as Li[Ni_1–x–yMn_xCo_y]O₂and Li[Ni_1−x−yCo_xAl_y]O₂. As Fe is abundant in nature, LiFePO₄is a low‐cost material. Moreover, stable structure of LiFePO₄imparts long service life and thermal stability. However, the practical implementation of LiFePO₄cathode in energy storage devices is impeded by its low energy density and high ionic/electrical resistance. Herein, the LiFePO₄electrode with high active material loading and low ionic/electrical resistance through the dry process is reported for the first time. The dry process not only enables the uniform distribution of the polymeric binders and conductive additives within the thick electrode but also inhibits the formation of cracks. Furthermore, the bridge‐like connection of polytetrafluoroethylene facilitates the insertion and extraction of Li ions to the LiFePO₄crystal. Hence, the dry‐processed LiFePO₄electrode with high areal capacity (7.8 mAh cm⁻²) exhibits excellent cycle stability over 300 cycles in full‐cell operation. In addition, it is demonstrated that the estimated energy density of prismatic cell with the dry‐processed LiFePO₄electrode is competitive with state‐of‐the‐art Li[Ni_1–x–yMn_xCo_y]O₂‐based battery.