<p>Due to the scarcity of rare strategic metals and their importance in advanced materials, the recovery of these metals from secondary resources has become more important. Recovering rare metals from typical hazardous waste—spent hydrotreating catalysts (SHC) in the petrochemical industry—not only contributes to reducing environmental pollution but also alleviates resource supply pressure. This paper presents a sulfuric acid roasting–ultrasonic leaching process, where ultrasonic-assisted technology enables the efficient recovery of vanadium (V), molybdenum (Mo), and nickel (Ni) within 15&#xa0;min of leaching, greatly enhancing process efficiency. Thermodynamic analysis, process analysis, and single-factor experiments further support the efficient conversion of valuable elements into soluble sulfates, providing a strong theoretical foundation for optimizing the recovery process. The process was optimized using response surface methodology (RSM) with the Box–Behnken design (BBD) to identify the key process conditions for efficient recovery of V, Mo, and Ni. The optimization significantly reduced H₂SO₄ dosage and lowered roasting and leaching temperatures, achieving the highest leaching efficiency while saving both energy and reagent consumption. Under the optimized conditions of a 350&#xa0;°C roasting temperature, 0.766 H₂SO₄ stoichiometric ratio, 71&#xa0;°C leaching temperature, and 0.6-mol/L H₂SO₄ concentration, the leaching efficiency of V, Mo, and Ni reached 94.26, 91.41, and 83.82%, respectively. Characterization analysis of the raw material, roasting product, and leaching residue further confirmed the effectiveness of the optimized process. This study provides innovative technical support for the efficient recovery of strategic metals from secondary resources, with promising potential for industrial applications.</p> Graphical Abstract <p></p>