Al2O3-supported Cu and Ni monometallic as well as Cu–Ni bimetallic catalysts were synthesized using a coprecipitation method and studied for the in-situ hydrogenation of furfural (FAL) with isopropanol as the solvent and hydrogen donor. The Cu–Ni bimetallic catalysts showed improved activity toward the production of 2-methylfuran (2-MF) and 2-methyl­tetrahydrofuran (2-MTHF) over that of monometallic catalysts. The results indicated that isopropanol exhibited better performance than methanol for the in-situ hydrogenation of FAL to produce 2-MF and 2-MTHF under the same conditions. The reaction conditions such as the copper–nickel ratios, catalyst loading amount, reaction temperature, and time were optimized. After the reaction was complete, the supported Cu–Ni bimetallic catalyst could be reused four times without a significant loss in catalytic activity.