A novel nanocomposite film synthesized from an inexpensive and easily accessible polymer such as poly (vinyl alcohol) (PVA), which is coated with nickel sulfide (NiS) and graphene oxide (GO), was obtained from used drinking-water bottles. The produced coated film was examined as a potential photocatalyst film for wastewater treatment promotion in a batch system for the removal of methylene blue (MB) and tetracycline (TC) antibiotics. The experimental results show that the presence of GO significantly increases the photocatalytic efficiency of NiS, and the MB and TC degradation results proved that the incorporation of GO with NiS led to a more than one-and-a-half-fold increase in the removal percentage in comparison with the NiS/PVA-coated film. After 30 min of illumination using GO/NiS/PVA-coated film, the removal efficiency reached 86% for MB and 64% for TC. The photodegradation kinetic rate followed the pseudo-first-order rate. Furthermore, the response surface methodology (RSM) model was utilized to study and optimize several operating parameters. The ideal circumstances to achieve 91% elimination of MB are 12 mg L−1 MB initial concentration, two lamps, and an illumination time of 15 min; however, to achieve 85% TC removal, 11 mg L−1 TC initial concentration, two lamps, and a 45 min illumination time should be used. The fabricated nanocomposite photocatalyst film seems to have promise for use in water purification systems.