Sequential infiltration synthesis (SIS) is an emerging vapor-phase synthetic route for the preparation of organic–inorganic composites. Previously, we investigated the potential of polyaniline (PANI)-InOxcomposite thin films prepared using SIS for application in electrochemical energy storage. In this study, we investigated the effects of the number of InOxSIS cycles on the chemical and electrochemical properties of PANI-InOxthin films via combined characterization using X-ray photoelectron spectroscopy, ultraviolet–visible spectroscopy, Raman spectroscopy, Fourier transform infrared spectroscopy, and cyclic voltammetry. The area-specific capacitance values of PANI-InOxsamples prepared with 10, 20, 50, and 100 SIS cycles were 1.1, 0.8, 1.4, and 0.96 mF/cm², respectively. Our result shows that the formation of an enlarged PANI-InOxmixed region directly exposed to the electrolyte is key to enhancing the pseudocapacitive properties of the composite films.