<p>In recent years, the in situ catalytic hydrodeoxygenation (HDO) of furfural (FA) to produce 2-methylfuran (2-MF) has attracted considerable research attention. However, most reported processes rely on expensive or corrosive hydrogen donors, such as secondary alcohols and formic acid, which limit their potential for large-scale application. In this study, a series of Al₂O₃-supported Ni-based catalysts was synthesized via a simple precipitation-hydrothermal method, and ethanol was employed as the economically viable hydrogen source for the HDO of FA. It was found that the introduction of yttrium (Y) during preparation significantly enhances the selectivity toward 2-MF. Over the optimal catalyst, Ni/Y₁Al₅, the conversion of FA exceeded 99.9% with a 2-MF yield of 95.6%. Characterization results revealed that the incorporation of Y could enhance dispersion of the active Ni species, modulate electron transfer between Ni and Y species and increase surface acid sites of Ni/Y₁Al₅. These beneficial factors collectively regulate the adsorption configuration of the C = O bond and enhance the adsorption of the intermediate (furfuryl alcohol, FOL) on Ni/Y₁Al₅, thereby promoting the formation of 2-MF. Furthermore, the Ni/Y₁Al₅ catalyst demonstrated excellent recyclability, with no significant loss in activity or selectivity over six reaction cycles.</p> Graphical Abstract <p></p>