The present study reports the feasibility of the synthesis of a novel porous composite adsorbent, prepared from olive stone activated carbon (OS400) and garnet (GA) mineral impregnations (referred to as OSMG). This composite (OSMG) was applied for its ability to adsorb a macromolecular organic dye. The composite’s structural characteristics were evaluated using various techniques such as Brunauer–Emmett–Teller (BET), Scanning Electron Microscopy equipped with Energy Dispersive X-ray spectroscopy (SEM–EDX), X-ray diffraction (XRD), and a Fourier transform infrared spectrometer (FT-IR). The specific surface area of the garnet (GA), (OS400), and (OSMG) were found to be 5.157 mg⋅g−1, 1489.598 mg⋅g−1, and 546.392 mg⋅g−1, respectively. The specific surface area of the new composite (OSMG) was promoted to enhance the adsorption of methylene blue (MB). Experiments were conducted under various conditions, including contact time, initial dye concentration, adsorbent dosage, pH, and temperatures. Data from these experiments were analyzed using several adsorption models including Langmuir, Freundlich, Temkin, and Dubinin-Radushkevich (D-R). The results indicated that, the adsorption fit best with the Freundlich model and that the adsorption process followed a pseudo-second-order kinetic mechanism. Additionally, the thermodynamic analysis indicated the adsorption of MB onto garnet(GA) adsorbents is endothermic, while the sorption onto (OS400) and (OSMG) is an exothermic and non-spontaneous process. The OSMG composite can be used for at least five cycles without significant loss of adsorptive performance, and can easily be separated from the water after treatment.