5-(Hydroxymethyl)furfural (HMF) and furfural (FF) have been identified as valuable biomass-derived fuel precursors suitable for catalytic hydrodeoxygenation (HDO) to produce high octane fuel additives such dimethyl furan (DMF) and methyl furan (MF), respectively. In order to realize economically viable production of DMF and MF from biomass, catalytic processes with high yields, low catalyst costs, and process simplicity are needed. Here, we demonstrate simultaneous coprocessing of HMF and FF over Cu−Ni/ TiO 2 catalysts, achieving 87.5% yield of DMF from HMF and 88.5% yield of MF from FF in a one pot reaction. The Cu−Ni/TiO 2 catalyst exhibited improved stability and regeneration compared to Cu/TiO 2 and Cu/Al 2 O 3 catalysts for FF HDO, with a ∼7% loss in FF conversion over four sequential recycles, compared to a ∼50% loss in FF conversion for Cu/Al 2 O 3 and a ∼30% loss in conversion for Cu/TiO 2. Characterization of the Cu−Ni/TiO 2 catalyst by X-ray photoelectron spectroscopy, scanning transmission electron microscopy, and H 2 −temperature-programmed reduction and comparison to monometallic Cu and Ni on Al 2 O 3 and TiO 2 and bimetallic Cu−Ni/Al 2 O 3 catalysts suggest that the unique reactivity and stability of Cu−Ni/TiO 2 derives from support-induced metal segregation in which Cu is selectively enriched at the catalyst surface, while Ni is enriched at the TiO 2 interface. These results demonstrate that Cu−Ni/TiO 2 catalysts promise to be a system capable of integrating directly with a combined HMF and FF product stream from biomass processing to realize lower cost production of liquid fuels from biomass.