In this work, three types of alumina‐supported bimetallic Ni−Cu catalysts [Ni−Cu/commercial non‐ordered mesoporous alumina (CMA), Ni−Cu/ordered MA (OMA), and Ni−Cu−OMA] were prepared via different fabrication strategies and investigated in the conversion of levulinic acid (LA) into γ‐valerolactone and 2‐methyltetrahydrofuran (2‐MTHF). This study employed characterization techniques and reactions to reveal the effects of the fabrication strategy on the activities of the catalysts. It was observed that the catalysts constructed on OM supports (Ni−Cu/OMA and Ni−Cu−OMA) displayed superior catalytic performance compared to those constructed on CM supports (Ni−Cu/CMA). Specifically, Ni−Cu−OMA, which was fabricated via the one‐pot evaporation‐induced self‐assembly strategy, exhibited the best catalytic performance, achieving a complete conversion of LA and a high selectivity of 73.0 % toward 2‐MTHF in a solvent‐free reaction environment. The promising activity of Ni−Cu−OMA was ascribed to the well‐dispersed active sites within the framework of the support, the enhanced metal‐support interaction, and the highly efficient exploitation of the synergistic effect between Ni and Cu. Detailed post‐characterization techniques were also employed to highlight the outstanding stability of Ni−Cu−OMA.