Polypyrrole (PPy) and polypyrrole-based gamma aluminum oxide (γ-Al 2 O 3 ) and gamma iron (III) oxide (γ-Fe 2 O 3 ) nanocomposites were synthesized via in situ electropolymerization methods Films were characterized via cyclic voltammetry (CV) and in situ spectroelectrochemistry methods such as in situ UV–Visible spectroscopy and in situ conductivity measurements. Polymer nanocomposite structures and morphologies were studied and characterized via Fourier transform infrared (FT-IR) spectroscopy, electrochemical impedance spectroscopy (EIS), energy dispersive X-ray spectroscopy (EDX), scanning electron microscopy (SEM), and transmission electron microscopy (TEM). According to the CV results of the nanocomposites, the separation of anodic and cathodic peak potential of the redox couples (ΔE) exhibited good reversibility with a positive potential shift compared with PPy during redox sweeps. The electrochemical properties of PPy, PPy/γ-Fe 2 O 3, and PPy/γ-Al 2 O 3 nanocomposite electrodes in a solution of H 2 SO 4 were studied via CV, galvanostatic charge–discharge, and EIS measurements to understand the pseudocapacitance that formed due to oxidation and reduction reactions over the double layer capacitance. Results for the nanocomposites revealed that they were very good candidates for supercapacitor applications, with higher specific capacitances, cyclic self-stabilities, and better rate capabilities than those of PPy films. The specific capacitance values of PPy/γ-Fe 2 O 3 (106 F/g) and PPy/γ-Al 2 O 3 (92 F/g) nanocomposites based on a three-electrode cell configuration from galvanostatic charge–discharge at a constant current density of 1 A/g were higher than that for PPy (75 F/g). [ABSTRACT FROM AUTHOR]