| Summary: | Although titanium dioxide has gained much attention as a sodium-ion battery anode material, obtaining high specific capacity and cycling stability remains a challenge. Herein, we report significantly improved surface chemistry and pseudocapacitive Na-ion storage performance of TiO<sub>2</sub> nanosheet anode in vinylene carbonate (VC)-containing electrolyte solution. In addition to the excellent pseudocapacitance (~87%), the TiO<sub>2</sub> anodes also exhibited increased high-specific capacity (219 mAh/g), rate performance (40 mAh/g @ 1 A/g), coulombic efficiency (~100%), and cycling stability (~90% after 750 cycles). Spectroscopic and microscopic studies confirmed polycarbonate based solid electrolyte interface (SEI) formation in VC-containing electrolyte solution. The superior electrochemical performance of the TiO<sub>2</sub> nanosheet anode in VC-containing electrolyte solution is credited to the improved pseudocapacitive Na-ion diffusion through the polycarbonate based SEI (coefficients of 1.65 × 10<sup>−14</sup> for PC-VC vs. 6.42 × 10<sup>−16</sup> for PC). This study emphasizes the crucial role of the electrolyte solution and electrode–electrolyte interfaces in the improved pseudocapacitive Na-ion storage performance of TiO<sub>2</sub> anodes.
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