A novel assembly method was used to prepare the sulfhydryl functionalized magnetic SBA-15 (SH-M-SBA-15). The physicochemical properties of SH-M-SBA-15 were characterized by TEM, XRD, EDS, FT-IR, BET, and VSM. Batch adsorption experiments were conducted to investigate the influence of initial uranium concentration, dosage of adsorbent, pH values, contact time, and temperature on the adsorption efficiency and behaviors. The adsorption types were analyzed from the aspects of kinetic, isotherms, and thermodynamic. The results show that the specific surface area of SH-M-SBA-15 is 316.67 m2/g, which is smaller than that of SBA-15 (692.18 m2/g). However, compared with SBA-15, SH-M-SBA-15 has more surface sulfhydryl functional groups. The addition of this group can improve the adsorption of uranyl ions by SH-M-SBA-15. The optimal adsorption conditions were adsorption dosage 40 mg/L, pH 6, temperature 35 °C, contact time 180 min, and initial uranium concentration 35 mg/L. Under this condition, the maximum adsorption amount of uranyl ion by SH-M-SBA-15 can reach 804.79 mg/g, which is much higher than the highest adsorption capacity of uranyl ion by SBA-15 (146.23 mg/g). The adsorption process was better depicted by the Langmuir isotherm model. The process was consistent with the quasi-second-order model. ΔG was negative and ΔH was positive, indicating spontaneous and endothermic adsorption.