In the present research, cellulose acetate (CA) and polyaniline (PANI) were combined to form CA/PANI films using the solution-casting method. This research aims to provide novel optical behavior for irradiated flexible CA/PANI sheets to be utilized in high-performing optical devices. The Fourier-transform infrared spectroscopy (FTIR), X-ray diffraction (XRD), and scanning electron microscope (SEM) were employed to effectively produce the CA/PANI samples. The argon fluence of [Formula: see text], [Formula: see text], and [Formula: see text][Formula: see text]ions/cm2 have been added to these films. The FTIR and XRD measurements showed that the ion treatment of CA/PANI films altered their functions and crystalline compositions. This indicates that the CA/PANI films were successfully prepared. The optical properties were measured using the UV–Vis technique in a wavelength of 200–1150[Formula: see text]nm. The Tauc relationship was used to estimate the band gap and Urbach energies of both bombarded and untreated films. In response to [Formula: see text], [Formula: see text], and [Formula: see text][Formula: see text]ions/cm2, CA/PANI exhibits a drop in band gap from 4.92[Formula: see text]eV to 4.45, 4.31, and 4.20[Formula: see text]eV, respectively. According to these results, the optical performance of the irradiated CA/PANI composite films was modified to be used in optoelectronics.