Magnetic granite (MG), a new and low-cost adsorbent, was prepared by the chemical co-precipitation of Fe2+ and Fe3+ using granite (G), which is a magmatic rock type. The adsorption of the Reactive Black 5 (RB5) dye from aqueous solutions on Fe3O4-modified granite was examined in a batch system. Fourier transform infrared spectroscopy (FTIR), scanning electron microscopy (SEM), energy-dispersive X-ray (EDX), X-ray fluorescence spectrometry (XRF), X-ray diffractometry (XRD), N2 adsorption−desorption, vibrating-sample magnetometry (VSM), and point-of-zero charge (pHpzc) analysis were used to characterize the prepared MG. Magnetic granite displayed significant magnetization and could be easily separated using external magnets. The maximum adsorption capacity was 29.85 mg/g at 298 K. According to kinetic and isothermal examinations, the pseudo-second-order model and Langmuir isothermal adsorption were the best fit for adsorption. It was found that the enthalpy change ΔH (kJ/mol) was −31.76, and the entropy change ΔS (kJ/mol) was 0.096 for a temperature change of 298−330 K. The ΔG° (kJ/mol) value was negative at all temperatures (298 K, −2.86 kJ/mol; 303 K, −2.85 kJ/mol and 313 K, −1.50 kJ/mol), indicating that the adsorption of RB5 on MG was spontaneous.