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As a versatile and valuable intermediate, furfuryl alcohol (FOL) has been widely used in manufacturing resins, vitamin C, perfumes, lubricants, plasticizers, fuel additives, biofuels, and other furan-based chemicals. This work developed an efficient hybrid strategy for the valorization of lignocellulosic biomass to FOL. Corncob (75 g/L) was catalyzed with heterogenous catalyst Sn-SSXR (2 wt%) to generate FAL (65.4% yield) in a deep eutectic solvent ChCl:LA–water system (30:70, v/v; 180 °C) after 15 min. Subsequently, the obtained FAL liquor containing FAL and formate could be biologically reduced to FOL by recombinant E. coli CF containing aldehyde reductase and formate dehydrogenase at pH 6.5 and 35 °C, achieving the FOL productivity of 0.66 g FOL/(g xylan in corncob). The formed formate could be used as a cosubstrate for the bioreduction of FAL into FOL. In addition, other biomasses (e.g., sugarcane bagasse and rice straw) could be converted into FOL at a high yield. Overall, this hybrid strategy that combines chemocatalysis and biocatalysis can be utilized to efficiently valorize lignocellulosic materials into valuable biofurans.