An aqueous hybrid electrochemical capacitor consisting of a capacitive manganese oxide (MnO2) positive electrode and a water-stable, protected Li negative electrode in near-neutral aqueous electrolyte (1.0 M Li2SO4, pH = 5.5) is demonstrated. Galvanostatic charge/discharge cycling tests were conducted with pouched cells, offering a cell voltage of 4.2 V with maximum specific energy of 753 W h kg−1 based on the positive electrode. The combination of a pseudocapacitive MnO2 positive and a Li negative electrode offers high specific charge and cell voltage, resulting in an aqueous hybrid electrochemical capacitor having exceptionally high specific energy.