Due to the rapid development of the livestock industry, particularly due to residual pharmaceutical antibiotics, environmental populations have been negatively affected. Herein, we report a ZnO/melamine-functionalized carboxylic-rich graphene oxide (ZFG) photocatalyst for visible light-driven photocatalytic degradation of tetracycline hydrochloride in aqueous solutions. The properties of the photocatalysts were evaluated by XRD, FTIR, XPS, Fe-SEM, HR-TEM, TGA, Raman spectroscopy, UV-Vis spectroscopy, zeta potential, and electrochemical measurements. The photocatalytic activity was measured using high-performance liquid chromatography. The photocatalytic properties of the ZFG photocatalyst evaluated against the tetracycline hydrochloride (TCH) antibiotic under visible light irradiation showed superior photodegradation of 96.27% within 60 min at an initial pH of 11. The enhancement of photocatalytic degradation was due to the introduction of functionalized graphene, which increases the light-harvesting capability and molecular adsorption capability in addition to minimizing the recombination rate of photogenerated charge carriers due to its role as an electron acceptor and mediator.