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The development of an active earth-abundant metal electrocatalyst for biomass-derived organic materials valorization can greatly benefit the growth of a sustainable biorefinery. Herein, we report a transition metal dichalcogenide catalyst, MoS2, as a great electrocatalytic hydrogenation catalyst in converting a highly versatile platform chemical furfural to furfuryl alcohol, with over 82.4% yield and 92.1% selectivity, and its catalytic performance surpassed those of 11 other base metal electrocatalysts. The durable layer of 1T-rich MoS2 was fabricated on a carbon cloth support via a novel seeded-solvothermal deposition, followed by a thermal treatment. Reaction mechanistic investigation via underpotential hydrogen desorption (HUPD) studies and substrate scope expansion showed that MoS2 delivered the mechanism in a stage-wise manner, where the reduction of the carbonyl occurred to yield a radical intermediate in the vicinity of the MoS2 catalyst, followed by an abstraction of a surface adsorbed hydrogen (Hads). The conversion of reactants benefited from the presence of electron-withdrawing substituents, and the product selectivity was inert to the influence of the substituents. The MoS2 can be prepared easily through electrocatalytic and solvothermal deposition. The resulting catalyst layer demonstrated great stability throughout the repeated application in bulk electrolysis. [ABSTRACT FROM AUTHOR]