Biomass-derived ethyl levulinate (EL) is currently deemed as a promising fuel bioadditive to improve (bio)diesel combustion performance without the sacrifice of its octane number. In this contribution, a range of Zr–Al bimetallic catalysts were prepared for the cascade conversion of furfural to EL by the integration of transfer hydrogenation and ethanolysis in ethanol. The ratio of Lewis to Brønsted acid sites (L/B) could be tuned by the ratio of Al2O3 to ZrO2 over SBA-15 support. Among these catalysts, Zr–Al/SBA-15(30:10) with appropriate L/B ratio of 2.25 exhibited an outstanding catalytic performance to give a furfural (FF) conversion up to 92.8% with a EL selectivity as high as 71.4% at 453 K in 3 h.