Currently, the catalytic transformation and utilization of biomass-derived compounds are of great importance to the alleviation of environmental problems and sustainable development. Among them, furfural alcohol derived from biomass resources has been found to be one of the most prospective biomass platforms for high-value chemicals and biofuels. Herein, high-surface-area ZrO₂ with abundant oxygen defects and surface acid–base sites was synthesized and used as a heterogeneous catalyst for the catalytic transfer hydrogenation of furfural into furfural alcohol using alcohol as a hydrogen donor. The as-synthesized ZrO₂ exhibited excellent catalytic performance with 98.2% FA conversion and 97.1% FOL selectivity, even comparable with that of a homogeneous Lewis acid catalyst. A series of characterization studies and experimental results revealed that acid sites on the surface of ZrO₂ could adsorb and activate the CO bond in furfural and base sites could facilitate the formation of alkoxide species. The synergistic effect of surface acid–base sites affords a harmonious environment for the reaction, which is crucial for catalytic transfer hydrogenation of furfural with high efficiency. Furthermore, the as-prepared ZrO₂ catalyst also exhibited a potential application for the efficient catalytic transfer hydrogenation of a series of biomass-derived carbonyl compounds.