SBA-15-supported ZrO2 were examined in the CTH reaction of levulinic acid and its esters. The catalyst efficiently produced GVL (∼95% yield) at 150 °C under 1.0 MPa of Ar. The catalytic activity far outperformed that of the conventional bulk ZrO2 catalyst. Highly-dispersed Zr4+-oxide with low-coordination geometry was the dominant active species. Based on NH3/CO2-TPD and in-situ FTIR results, a plausible reaction mechanism was proposed.