A series of layered double hydroxides (LDHs) with different Cu/Co ratio were prepared according to the coprecipitation method and used as catalyst precursors for higher alcohols synthesis. The prepared samples were characterized by XRD, TPR, SEM, TEM and BET techniques. After calcination, LDHs were transformed into a mixture of CuO, Co3O4, CuCo2O4 and alumina, and these oxides were mixed uniformly with size in several nanometers. For the sample with ratio of Cu/Co = 1/2, copper and cobalt species are mainly in CuCo2O4 phase. In the reduction process, the superior mixed copper and cobalt species in nanoscale were reduced to Cu-Co alloy, which was confirmed by XRD and TEM results. The prepared bimetallic catalysts showed high activity, good stability and much high selectivity to C2+ alcohols. Over the best catalyst, CO conversion of 51.8%, selectivity to alcohols of 45.8% and 94.3 wt. % of C2+OH in the total alcohols were obtained at 250ºC, 3MPa and GHSV of 3900 mL (gcat h) -1 .