Herein, we report that highly dispersed copper–cobalt mixed metal/metal oxide nanoparticles embedded into three-dimensional porous carbon were highly catalytic active nanocomposites for transforming bioderived furfural (FAL) to cyclopentanone (CPO) via aqueous-phase hydrogenation/rearrangement. This simple and efficient catalyst was prepared by controlled pyrolysis procedure using glucose as the carbon source at 500 °C under N2 atmosphere. Characterization of the as-prepared CuCo0.8@C-500 catalyst by XRD, STEM, SEM, TEM, and XPS suggested that there was a synergism between copper and cobalt. Under an extremely low H2 pressure (0.5 MPa), 90.2% yield of CPO could be attained at 150 °C. In addition, the sample could be recycled for several times without decrease in catalytic activity. Two critical reaction intermediates of furfuryl alcohol (FOL) and 2-cyclopentenone (2-CPE) were detected in the tandem catalytic process. These results demonstrated that this synthetic strategy represented a simple and effective way for utilization of inexpensive biomass resources to obtain some valuable chemicals.