3D architecture is fabricated by atomically thin 2D sheets of GO and ZrO2 nanoparticle as the building blocks using a facile one-pot chronopotentiometry method. Highly stable, conductive additive and binder free supercapacitor electrode shows superior electrochemical properties. The synergistic effect between the components and the tailored morphology enhances the electrochemical performance and material stability. Possible correlation of the structure and electrochemical performance of the 3D ternary composite is substantiatedusing a fully atomistic molecular dynamics (MD) simulation and DFT calculations.