A high-performance Cu–Ni bimetallic catalyst supported on Zr–Al oxides was fabricated for catalyzing the transfer hydrogenation of levulinate esters to γ-valerolactone (GVL) under mild conditions. The Cu₂Ni₁/Zr₃Al₇O_z catalyst provided the highest ethyl levulinate conversion of 99% with 96.8% GVL yield at 150 °C in 8 h employing 2-butyl alcohol (2-BuOH) as the hydrogen source. The catalyst was also used successfully for the catalytic transfer hydrogenation (CTH) of a series of levulinate esters. Moreover, the catalyst still retained high activity after recycling for 4 times. The outstanding catalytic performance and selectivity of Cu₂Ni₁/Zr₃Al₇O_z, together with its low-cost nature, make it have great application potential as a catalyst for the fabrication of GVL on a large scale in industry.