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Carbon nanotube (CNT) intercalated‐bismuth oxide (CNT‐Bi2O3)/polyvinylidenefluoride (PVDF) composites are synthesized via sonication and roasting process. The phase structure, bonding, and morphology of CNT‐Bi2O3/PVDF composite are characterized using X‐ray diffraction (XRD), Fourier transform infrared spectrum (FTIR), and scanning electron microscopy (SEM). The capacitance and dielectric constant of the composite electrodes are studied by impedance analyzer. The capacitance and stability of CNT‐Bi2O3/PVDF composite are found to be increased on increasing concentration of Bi2O3 in PVDF composite. These results show that CNT‐Bi2O3/PVDF composite is a very promising electrode material for high‐performance super capacitors.