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In cross-coupling of biomass-derived acetone and alcohols contributing to the production of carbon-elongated chemicals and fuels, the essential catalyst components are metal dispersion for alcohol dehydrogenation and, more importantly, basicity for carbon–carbon coupling. Herein, we report the potential of co-precipitated praseodymia–zirconia solid solution (Pr₂Zr₂O₇) as a support of Cu catalyst for the conversion of acetone and butanol into C₇ and C₁₁ products. Cu/Pr₂Zr₂O₇ exhibits a high yield of C₇ and C₁₁ (ca. 84%) compared to Cu/ZrO₂ and Cu/PrO_1.83. Moreover, it is robust under the employed solvent-free conditions owing to a solid solution of Pr₂Zr₂O₇ compared to PrO_1.83 showing phase transition to PrOHCO₃. It is also tolerant to up to 5 wt % water of the reactant mixture, recyclable once adequate post-treatment is employed after the reaction, and can convert the acetone–butanol–ethanol mixture into C₅–C₁₁ products at the nearly equivalent yield (82%) to the acetone–butanol mixture. Therefore, the Cu/Pr₂Zr₂O₇ reported herein is an efficient catalyst for the coupling of acetone with linear aliphatic alcohols into biofuel precursors.