Abstract: This study explores the controllable synthesis of CuAlO₂ using copper hydroxide and pseudo-boehmite powders as raw materials via a simple solid-phase ball milling method, along with its catalytic performance investigation in methanol steam reforming (MSR). Various catalysts were prepared under different conditions, such as calcination temperature, calcination atmosphere, and heating rate. Characterization techniques including BET, XRD, XPS, SEM, and H₂-TPR were employed to analyze the samples. The results revealed significant effects of calcination temperature on the phase compositions, specific surface area, reduction performance, and surface properties of the CA-T catalysts. Based on the findings, a synthesis route of CuAlO₂ via the solid-phase method was proposed, highlighting the importance of high calcination temperature, nitrogen atmosphere, and low heating rate for CuAlO₂ formation. Catalytic evaluation data demonstrated that CuAlO₂ could catalyze MSR without pre-reduction, with the catalytic performance of CA-T catalysts being notably influenced by calcination temperature. Among the prepared catalysts, the CA-1100 catalyst exhibited the highest catalytic activity and stability. The findings of this study might be useful for the further study of the catalytic material for sustained release catalysis, including the synthesis of catalytic materials and the regulation of sustained release catalytic performance.