Design of active and selective supported catalysts is critical for developing new tandem processes for upgrading biomass-derived alcohols. Hydrogen-free upgrading alcohols to liquid hydrocarbons is desirable for producing drop-in fuel substitutes, but direct and atom-economical processes are yet to be reported. Here we report a novel alcohol upgrading and deoxygenation cascade that meets these criteria. This hydrogen-free cascade is catalyzed by multifunctional Pd catalysts, whose supports feature a range of acid-base properties: primarily basic MgO, acidic Al2O3 and Mg-Al hydrotalcite (HT) with a combination of Lewis acidic and basic sites. The impact of support selection on selectivity offers insights into the design principles for next-generation catalysts for this process and related transformations.