Reduced graphene oxide-carbon nanotube (rGO-CNT) and anatase TiO2-Li4Ti5O12 (ATO-LTO) composite electrodes were synthesized via electrostatic spray deposition (ESD) and analyzed as cathode and anode vs. lithium, respectively. The rGO-CNT and ATO-LTO electrodes were able to deliver discharge capacities of ca. 63 mAhg -1 and 95 mAhg -1 , respectively for a current rate of 0.1 Ag -1 with superior rate capability and cycle stability. Post electrode analyses, lithium-ion hybrid electrochemical capacitors (Li-HEC) were constructed comprising a prelithiated ATO-LTO anode and an activated rGO-CNT cathode in a carbonate based 1M LiPF6 salt electrolyte. The Li-HEC cells were stable for a cell potential of 0.05-3V and were able to deliver a maximum gravimetric energy density of 33.35 Whkg -1 and a maximum power density of 1207.4 Wkg -1 , where the cell parameters were normalized with the total mass of the anode and cathode active materials. Furthermore the Li-HEC cells were able to retain ~77% of the initial capacity after 100 cycles. The superior Li-HEC performance is attributed to the utilization of a prelithiated lithium-intercalating anode and a double layer cathode in an asymmetric configuration. The feasibility of using a low-cost, facile process like ESD was therefore shown to produce high performance Li-HECs.