Developing environmentally friendly methods for reducing graphene oxide (GO) is essential. This study investigates the surface modification and reduction of GO films using 200 eV argon ion (Ar+) beam irradiation. X-ray Photoelectron Spectroscopy (XPS) analysis reveals significant chemical changes on the GO surface. GO was irradiated with a 200 eV Ar+beam for varying times (0–80 s). XPS survey spectra showed the presence of carbon and oxygen, with an increasing carbon atomic percentage over time. High-resolution XPS spectra of C 1s revealed peaks corresponding to sp2, C–OH, O–C–O, CO, and O–CO bonds. In the O 1s spectra, CO, O–C–O, and C–OH groups were observed. Upon irradiation, the CO peak consistently decreased, the O–C–O peak fluctuated, and the C–OH peak increased, indicating effective reduction of CO groups, dynamic changes in O–C–O functionalities, and the formation of additional C–OH groups. The C/O ratio increased from ∼2.4 to 2.7, underscoring the reduction process and enhanced carbon content. This method proves to be an efficient approach for producing reduced graphene oxide (rGO) with improved properties for advanced applications.