With a low cost and high volumetric capacity, rechargeable magnesium batteries (RMBs) have emerged as promising candidates for post-lithium ion batteries. The kinetically sluggish Mg 2+ insertion/ extraction in the host lattice and the anode/electrolyte incompatibility render the battery irreversible in some instances and restrict the commercial applications. In this work, we replace the conventional electrolyte with a dual layer of liquid and polymer electrolyte onto the cathode and anode, respectively, and investigate the structural, electrical, and electrochemical properties. It exhibits a remarkable Mg-ion conductivity up to 4.62 × 10 −4 S cm −1 at 55 °C, a high transfer number (t Mg 2+ = 0.74), low overpotential, and relatively stable Mg stripping and plating during the initial cycles. Furthermore, this work uses an unconventional electrode, BaTiO 3 (BTO), to demonstrate the performance of Mg batteries and track the structural and electrochemical changes. The quasi-solid-state Mg batteries fabricated with premagnesiation and thermally treated BTO cathode materials show good electrochemical performance. The approaches herein may provide new directions for exploiting high-performance Mg batteries through the perovskite structure cathode and functional dual electrolyte.

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