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Summary Supercapacitors are the electrochemical capacitors with high energy density. In this study, first, carbon aerogels (CAs) having different structural properties (surface areas and pore diameters) were synthesized. Their polypyrrole (PPy) composites on these CAs were synthesized via oxidative polymerization. The change in the capacitive properties depending on both different CA structural properties and PPy addition was determined. The materials were characterized by Fourier Transform Infrared Spectrocope (FTIR), X‐ray diffraction (XRD), nitrogen adsorption/desorption isotherms with Brunauer, Emmett and Teller (BET) method, scanning electron microscope (SEM), transmission Electron Microscope (TEM), elemental analysis and thermal gravimetric analysis (TGA) methods. Specific capacitances of the nanocomposites were determined by cyclic voltammetry (CV) method for fresh electrode and the aged electrode after 1000 cycles. It was observed that the specific capacitance of the composite obtained with the addition of PPy to the first type of carbon aerogel (CA1) material varies significantly and increased from 147 F g−1 (CA1) to 231 F g−1 (CA1/PPy).