One-pot catalytic conversion of raw woody biomass into valuable chemicals and fuels is a promising strategy for relieving energy depletion. Here, we proposed an efficient catalyst combining highly dispersed and ultrafine platinum nanoparticles on ceria doped with Cr, enabling nearly complete conversion, and obtaining value-added chemicals and bio-fuel with high energy density. The key part of our approach lies on the flexible utilization of a synergetic catalysis system consisting of a redox potential CeCrO2−x, balanced acid-base properties and strong metal-support interaction. Abundant oxygen vacancies and enhanced wettability have been achieved by properly doping of Cr. Under nitrogen atmosphere, the catalyst still shows excellent conversion performance, not only can hydrogen transfer be achieved by using the “borrowed” hydrogen, but also the Guerbet reaction can suppress the formation of intractable chars. Moreover, alcoholophilicity facilitates the dispersion of the catalyst particles in ethanol, leading to higher mass transfer efficiency. The catalyst can be separated facilely and reused three times without obvious deactivation.