The synthesis of 2,5-dimethylfuran (DMF) from 5-hydroxymethylfurfural (HMF) is a highly attractive route to a renewable fuel. Herein, we propose that non-noble Co-based catalysts derived from layered double hydroxides (LDHs) can efficiently convert HMF into 2,5-dimethylfuran (DMF). Homogeneous elemental distributions of the Co-containing LDH precursors facilitate good dispersion of Co and the metal oxide species and also strong interaction between them on the resulting catalyst, therefore exhibiting superior reactivity under mild condition. Through fine modulation of the metal nanostructure, a high DMF yield of 74.2% at a mild reaction temperature of 130 degrees C with 0.7 MPa H-2 can be achieved. The well-distributed Co sites on the metal-support interface are deduced to be responsible for the efficient HMF and H-2 activations. The Co-based catalysts present good active both on hydrogenation of C=O and C-O, which have great potential for biomass utilization.