In this work, zinc oxide (ZnO)/granular activated carbon (GAC) composites at different ZnO concentrations (0.25M-ZnO@GAC, 0.5M-ZnO@GAC, and 0.75M-ZnO@GAC) were prepared by an in-situ hydrothermal method and demonstrated synergistic photocatalytic degradation and adsorption of rhodamine B (RhB). The thermal stability, morphological structure, elemental composition, crystallographic structure, and textural properties of developed catalysts were characterized by thermal gravimetric analysis (TGA/DTG), scanning electron microscopy equipped with energy dispersive-x-ray (SEM-EDS), X-ray diffraction (XRD), and Brunauer-Emmett-Teller (BET) analysis. The successful loading of ZnO onto GAC was confirmed by SEM-EDS and XRD analysis. The BET surface areas of GAC, 0.25M-ZnO@GAC, 0.5M-ZnO@GAC, and 0.75M-ZnO@GAC were 474 m2/g, 450 m2/g, 453 m2/g, and 421 m2/g, respectively. The decrease in GAC could be attributed to the successful loading of ZnO on the GAC surface. Notably, 0.5M-ZnO@GAC exhibited the best photocatalytic degradation efficiency of 82% and 97% under UV-A and UV-C light over 120 min, attributed to improved crystallinity and visible light absorption. The photocatalytic degradation parameters revealed that lowering the RhB concentration and raising the catalyst dosage and pH beyond the point of zero charge (PZC) would favor the RhB degradation. Photocatalytic reusability was demonstrated over five cycles. Scavenger tests revealed that the hydroxyl radicals (•OH), superoxide radicals (O2-•), and photoinduced hole (h+) radicals play a major role during the RhB degradation process. Based on the TOC results, the RhB mineralization efficiency of 79.1% was achieved by 0.5M-ZnO@GAC. Additionally, GAC exhibited a strong adsorptive performance towards RhB, with adsorption capacity and the RhB removal of 487.1 mg/g and 99.5% achieved within 90 min of equilibrium time. The adsorption characteristics were best described by pseudo-second-order kinetics, suggesting chemical adsorption. This research offers a new strategy for the development of effective photocatalyst materials with potential for wider wastewater treatment applications.