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Calender process is important to improve the mechanical and electrochemical properties of cathode materials. To explore pressure effect on structure and resistance of electrode powder, the morphology and surface area of lithium cobalt oxide (LCO) powder under different pressure are investigated. Meanwhile, the real‐time stress, density, and conductivity of LCO powder upon compaction are tested by a self‐made detection system. Moreover, the battery performance of LCO powder after compaction is compared in coin cells. This work elucidates the relationship between compaction density, powder resistance, and electrochemical performance of cathode materials for lithium‐ion batteries. [ABSTRACT FROM AUTHOR]