A polybenzopyrrole@nickel oxide (Pbp@NiO) nanocomposite was synthesized by an oxidative chemical one-pot method and tested as an active material for hybrid electrodes in an electrochemical supercapattery device. The as-prepared composite material exhibits a desirable 3D cross-linked nanostructured morphology and a synergistic effect between the polymer and metal oxide, which improved both physical properties and electrochemical performance. The unprocessed material was characterized by X-ray diffraction, FTIR and UV–Vis spectroscopy, scanning electron microscopy/energy disperse X-ray analysis, and thermogravimetry. The nanocomposite material was deposited without a binder on gold current collectors and investigated for electrochemical behavior and performance in a symmetrical two- and three-electrode cell setup. A high specific capacity of up to 105 C g−1 was obtained for the Pbp@NiO-based electrodes with a gravimetric energy density of 17.5 Wh kg−1, a power density of 1,925 W kg‑1, and excellent stability over 10,000 cycles.