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Polyaniline (PANI), which is highly conductive, could be used in various applications, including energy storage, photocurrent production, and sensor devices. In order to obtain pure and high-performance PANI nanofibers films, aniline was electropolymerized into PANI films using two electrochemical techniques onto an indium tin oxide coated glass substrate (ITO). Scanning electron microscopy (SEM), X-ray photoelectron spectroscopy (XPS), ultraviolet–visible spectroscopy (UV–vis), and electrochemical photocurrent spectroscopy were used to analyze the thin films of PANI nanofibers (EPS). SEM studies were shown the formation of PANI nanofibers with widths ranging from 50 to 150 nm. The PANI composition, which consists of the chemical elements carbon (C), oxygen (O), and nitrogen (N), is also confirmed by XPS (N). PANI films have also been investigated for their potential as electrochromic materials with potential uses in smart windows and color-changing devices like electrochromic devices. The results demonstrated the high performance of the photoresponse of PANI films made using electrochemical synthesis via cyclic voltammetry (CV) and chronoamperometry (CA) methodologies. The findings also show that the PANI films by (CV) have a better response than the PANI films by (CA), where the photoresponse to the current reaches from 0.1 mA/cm2 to 0.4 mA/cm2 with the applied potentials, in contrast to the films of the PANI (CA), which had the highest response of 0.2 mA/cm2. These findings could be considered promising for photocatalysis, photodegradation, and optoelectronic applications.