Designing efficient and facile recoverable catalysts is desired for sustainable biomass valorization. This work reports the one-pot synthesis of a novel magnetic Fe(NiFe)O4-SiO2 nanocatalyst for hydrogenation of biomass-derived furfural into valuable furfuryl alcohol. Various techniques were used to systematically analyze the physicochemical properties of the Fe(NiFe)O4-SiO2 nanocatalyst. Vibrating sample magnetometer analysis reveals low coercivity of Fe(NiFe)O4-SiO2 (6.991 G) compared with that of Fe3O4-SiO2 (27.323 G), which is attributed to highly dispersed Ni species in the Fe(NiFe)O4-SiO2 catalyst. HRTEM images indicated the nanosized nature of the Fe(NiFe)O4-SiO2 catalyst with an average diameter of ∼14.32 nm. The Fe(NiFe)O4-SiO2 catalyst showed a superior BET surface area (259 m2/g), which is due to the formation of nanosized particles. The magnetic Fe(NiFe)O4-SiO2 nanocatalyst shows a remarkable performance with 94.3 and 93.5% conversions of furfural and ∼100% selectivity of furfuryl alcohol at 90 °C and 20 H2 bar and 250 °C and 5 H2 bar, respectively. Using heptane as a solvent, the effect of temperature, pressure, reactant amount, and catalyst loading were investigated to optimize the reaction conditions. A probable mechanism via a non-hydrogen spillover route was proposed for the hydrogenation of furfural to furfuryl alcohol over the magnetic Fe(NiFe)O4-SiO2 nanocatalyst. The efficiency of the magnetic Fe(NiFe)O4-SiO2 nanocatalyst is attributed to highly dispersed nickel species, which plays a key role in the dissociation of H2 into a proton and a hydride in the furfural hydrogenation. The superior performance of the magnetic Fe(NiFe)O4-SiO2 nanocatalyst, along with the advantages of low cost and easy recoverability, could make it a new appealing catalyst in various selective hydrogenation reactions. © 2016 American Chemical Society.