A novel preparation method for bimetallic nickel-indium alloy catalysts supported on amorphous alumina (Ni-In(x)/AA; x = Ni/In molar ratio) catalysts has been developed and evaluated for the highly selective hydrogenation of biomass-derived furfural. Ni-In(x)/AA catalysts were obtained via the hydrothermal treatment of Raney® nickel supported on aluminium hydroxide (R-Ni/AlOH) and an InCl2·H2O solution in an ethanol/H2O mixture at 423 K for 2 h, followed by reduction with H2 at 573–873 K for 1.5 h. The formation of Ni-In alloy phases such as Ni3In2, Ni3In, Ni2In, and NiIn in Ni-In(2.0)/AA was clearly observed after reduction with H2 at 873 K for 1.5 h. Ni-In(2.0)/AA contained a Ni2In alloy as the major phase, which exhibited the best catalytic performance for the selective hydrogenation of furfural into furfuryl alcohol and was stable for at least five consecutive reaction runs.