Enhanced Production of Biomass‐Derived δ‐Valerolactone Through Coupled Hydrogenation and Dehydrogenation Pathways

δ‐Valerolactone (DVL) is a monomer with promising applications in the production of biodegradable and biocompatible polymers. This study addresses, for the first time, a sustainable route for DVL production by coupling liquid‐phase furfural (FF) hydrogenation with 1,5‐pentanediol (1,5‐PDO) dehydrogenation, where FF acts as a hydrogen acceptor. In addition, the potential regeneration of 1,5‐PDO from FF, thereby contributing to the closure of the material cycle, is evaluated. For this purpose, Cu─Ni─Al hydrotalcites‐derived catalysts with varying Cu:Ni ratios were prepared. Comprehensive physicochemical characterization revealed that Cu:Ni ratio strongly influences the catalyst structure and the textural properties, significantly affecting the catalytic performance of the catalysts. Catalytic tests allowed for obtaining substrate conversion values above 90% and DVL yields over 65%, demonstrating that hydrogen‐transfer coupling significantly promotes DVL production under liquid‐phase conditions. Kinetic studies based on a simplified model provided preliminary estimates of the apparent activation energies of 120 kJ mol ⁻¹ for FF hydrogenation and 80 kJ mol ⁻¹ for 1,5‐PDO dehydrogenation, highlighting the potential of dual catalytic systems for biomass valorization and the production of sustainable monomers under liquid‐phase conditions.