attract increasing attention. [2] However, the progress in Ca 2+ -ion batteries is very sluggish due to multiple difficulties. One major challenge is the lack of applicable electrolytes that can provide a proper function for the stripping and plating of calcium metal. [3] Another challenge is the difficulty in realizing proper cathode host materials. As a matter of fact, there are substantial differences in the interaction behavior between the divalent Ca 2+ -ion and that of the monovalent Li + -ion. [4] Therefore, neither theoretical guidance nor practical experience with Li + -ion intercalation cathode materials may be straightforwardly adopted for the development of Ca 2+ -ion batteries.In an early stage, V 2 O 5 has been explored as an intercalation-type cathode for Ca 2+ -ion batteries, but the utilization of Ca is very low. [5] Ca-SOCl 2 battery systems have also been exploited, but the utilization of the SOCl 2 electrode is very low due to the passivation of the electrode. [6] In recent years, an intercalation cathode CaCo 2 O 4[7] and various conversion-type hexacyanoferratebased cathodes [8] have been investigated. The Ca 2+ -ion cells demonstrated with these cathode materials have shown interesting performances. However, the capacity of these materials is intrinsically low. Nonaqueous metal-sulfur batteries based on a sulfur cathode chemistry have recently been considered as a promising solution for the development of nextgeneration electrochemical energy storage technologies. [9] Sulfur can facilitate a 2-electron charge transfer and theoretically deliver a high gravimetric capacity of 1672 mA h g −1 . In addition to the primary emphasis on lithium-sulfur (Li-S) batteries, [10] sodiumsulfur batteries, [11] magnesium-sulfur (Mg-S) batteries, [12] potassium-sulfur batteries, [13] and aluminum-sulfur (Al-S) batteries [14] have also received significant attention. However, to date, there has been only one study on calcium-sulfur (Ca-S) batteries, and the Ca-S cells demonstrated in that study were not reversible. [15] Furthermore, the Ca-S cell showed a low discharge voltage due to lack of an effective electrolyte.Herein, we present, for the first time, a reversible Ca-S battery enabled by a lithium-ion mediation strategy. The Ca-S battery is developed with a hybrid electrolyte comprised of a mixture of lithium and calcium ions. In addition to enabling the reversibility of Ca-S chemistry, the use of Li + -ion mediated electrolyte enhances the ionic charge transfer, thus both utilization of the active sulfur cathode and the discharge voltage of the Ca-S batteries are significantly improved.Calcium represents a promising anode for the development of high-energydensity, low-cost batteries. However, a lack of suitable electrolytes has restricted the development of rechargeable batteries with a Ca anode. Furthermore, to achieve a high energy density system, sulfur would be an ideal cathode to couple with the Ca anode. Unfortunately, a reversible calciumsulfur (Ca-S) battery has not yet been reported. Herein,...