In this study, chemoenzymatic synthesis of furfuryl alcohol from biomass (e.g., corncob, bamboo shoot shell, and rice straw) was attempted by the tandem catalysis with Lewis acid (SnCl or solid acid SO/SnO-bentonite) and biocatalyst in one-pot manner. Compared with SnCl, solid acid SO/SnO-bentonite had higher catalytic activity for converting biomass into furfural, which could be biologically converted into furfuryl alcohol with Escherichia coli CCZU-H15 whole-cell harboring reductase activity. Sequential catalysis of biomass into furfural with SO/SnO-bentonite (3.0 wt%) at 170 °C for 0.5 h and bioreduction of furfural with whole cells at 30 °C for 4.5 h were used for the effective synthesis of furfuryl alcohol in one-pot media. Corncob, bamboo shoot shell, and rice straw (3.0 g, dry weight) could be converted into 65.7, 50.3, and 58.5 mM furfuryl alcohol with the yields of 0.26, 0.25, and 0.23 g furfuryl alcohol/(g xylan in biomass) in 40 mL reaction media. Finally, an efficient process of recycling and reusing of SO/SnO-bentonite catalyst and immobilized whole-cell biocatalyst was developed for the chemoenzymatic synthesis of furfuryl alcohol from biomass in the one-pot reaction system.