Ca‐ion based devices are promising candidates for next‐generation energy storage with high performance and low cost, thanks to its multielectrons, superior kinetics, as well as abundance (2500 times lithium). Because of the lack of an appropriate combination of suitable electrode materials and electrolytes, it is unsuccessful to attain a satisfactory performance on complete Ca‐ion energy storage devices. Here, the multiion reaction strategy is defined to construct a complete Ca‐ion energy storage device and a capacitor–battery hybrid mechanism is deliberately adopted. Profiting from the elaborate design, it exhibits a high reversible capacity of 92 mAh g−1, unmatchable rate capability, and a high capacity retention of 84% over 1000 cycles under room temperature, which is the best performance of reported Ca‐based energy storage devices. [ABSTRACT FROM AUTHOR]