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A challenge in developing high-performance lithium batteries requires a safe technology without flammable liquid electrolytes. Nowadays, two options can satisfy this claim: all-solid-state batteries and aqueous-electrolyte batteries. Commercially available Li-ion batteries utilize non-aqueous electrolytes (NAE) owing to a wide potential window (>3 V) that achieves high energy density but pose serious safety issues due to the high volatility, flammability, and toxicity of NAE. On the contrary, aqueous electrolytes are non-flammable, low-toxic, and have a low installation cost for humidity control in the production line. In this scenario, we develop a new aqueous rechargeable Li-ion full-cell composed of high-voltage cathode material as LiCoO2 (LCO) and a safe nanostructured anode material as Li2TiO3 (LTO). Both pure-phase LTO and LCO nanopowders are prepared by hydrothermal route and their structural and electrochemical properties are studied in detail. Simultaneously, the electrochemical performances of these electrodes are tested in both half- and full-cell configurations in presence of saturated 1 mole L−1 Li2SO4 aqueous electrolyte medium. Pt//LCO and Pt//LTO half-cells deliver high discharge capacities of 142 and 133 mAh g−1 at 0.5 C rate with capacity retention of ~95% and 94% after 50 cycles with a Coulombic efficiency of 98.25% and 99.89%, respectively. The electrochemical performance of a LTO//LCO full cell is investigated for the first time. It reveals a discharge capacity of 135 mAh g−1 at 0.5 C rate (50th cycle) with a capacity retention of 94% and a Coulombic efficiency of 99.7%.