Nickel is a promising catalyst for the hydrogenation of furfural (FA) into furfuryl alcohol (FOL) and tetrahydrofurfuryl alcohol (TFOL). However, slow H* desorption and low catalytic selectivity limit its practical application. Herein, we employed an alloying strategy to tailoring the d-band center of Ni by Cu for efficient and selective catalytic hydrogenation of furfural. A series of Ni-Cu alloy catalysts (NiCux/C) were prepared by pyrolyzing NiCux-BTC (a MOF containing Cu and Ni) precursors. Theoretical calculation demonstrates that Ni exhibits a downshifted d-band center once alloyed by Cu. This change can not only promote the desorption of H from Ni surface to improve the catalytic activity but also thermodynamically favor the transformation of adsorption orientation of FA (from a flat orientation on Ni to a tilted one on Ni-Cu alloy) to enable the selective conversion of FA into FOL or TFOL on demand. NiCu0.33/C catalyst exhibits enhanced activity and selectivity for FA hydrogenation compared to pure Ni and Cu. (C) 2020 Elsevier Inc. All rights reserved.