In-situ hydrothermal method is employed to synthesize graphene/zirconium oxide composite from respective precursors graphene oxide and zirconium oxy-nitrate. In this method, the graphene oxide is reduced itself to graphene and simultaneously metal oxide gets anchor on the graphene sheets. A novel method is also developed for the preparation of vertically aligned tunable polyaniline on the graphene/zirconium oxide nanocomposite, which leads to achieve high surface area (207.1 m2 g−1), high electrical conductivity (70.8 S cm−1), high specific capacitance (1359.99 Fg−1 at 1 mV s−1), and high electrochemical performances as supercapacitor electrode materials. This vertically aligned conducting polymer gets easy contact with electrolyte ions and provides numerous redox active sites during charging and discharging. Moreover, such a simple and low cost assembly approach can be a pioneer for the large-scale production of various functional architectures for energy storage and conversions.