This study presents a novel photocatalytic system for photocatalytic degradation of Eriochrome black-T (EBT) dye via green light-emitting diode (LED) light exposure. This photocatalyst is comprised of nanoscale components, i.e., poly- (vinyl alcohol) (PVA), magnetic iron oxide nanoparticles (Fe3O4 NPs), gold NPs (Au NPs), and zinc oxide nanorods (ZnO NRs), rendering an active high surface area. The most highlighted property from the structural facet is the superparamagnetic behavior of Fe3O4 NPs, which provides a facile collection of magnetic photocatalyst NPs from the reaction flask and is successfully recycled eight times without considerable reduction in catalytic behavior. Briefly, the photocatalytic degradation at its highest efficiency reached 51.4% (10 ppm dye solution, 5.0 mL) and 64.75% (8 ppm dye solution, 5.0 mL) utilizing 10 mg of the designed photocatalyst (formulated as Fe3O4@PVA−Au/ZnO), a magnetic photocatalytic system under green LED light (7 W, 526 nm) exposure for 60 min. Besides, the photocatalytic degradation mechanism of the EBT dye by the as-prepared photocatalyst was proposed. Based on the obtained results, the presented photocatalytic method was recommended for scaling up and large-scale exploitation for the purification of the water resources.