A study reports a reductive catalytic approach using a bifunctional Pt/H-MOR catalyst to depolymerize technical lignin, achieving a 2–11 times higher monomer yield than previously reported. The method selectively cleaves various C–C bonds in lignin, including aryl–aryl, aryl–alkyl, and alkyl–alkyl linkages, under mild conditions. The catalyst's Brønsted acid sites facilitate cleavage of aryl–alkyl bonds, while Pt hydrogenates aryl moieties and introduces double bonds in alkyl ones, followed by acid-catalyzed β-scission. This approach significantly improves monomer yields, with the best results constituting a 58–409% increase over conventional maximum monomer yields. The study demonstrates the utility of this method in valorizing various lignins, achieving a 54.0% monomer yield through reductive C–C and C–O cleavage. A techno-economic analysis shows the potential of this method for producing gasoline- and jet-range cycloalkanes and aromatics, while a life-cycle assessment confirms its potential for CO₂-neutral fuel production. The approach is effective for upgrading oligomers obtained by aldehyde-assisted fractionation or RCF from lignocellulosic biomass, as well as various technical lignins, underpinning the broad utility of the method. The study highlights the importance of C–C bond cleavage in lignin valorization and demonstrates the feasibility of a CO₂-neutral lignin biorefinery aimed at fuel production.A study reports a reductive catalytic approach using a bifunctional Pt/H-MOR catalyst to depolymerize technical lignin, achieving a 2–11 times higher monomer yield than previously reported. The method selectively cleaves various C–C bonds in lignin, including aryl–aryl, aryl–alkyl, and alkyl–alkyl linkages, under mild conditions. The catalyst's Brønsted acid sites facilitate cleavage of aryl–alkyl bonds, while Pt hydrogenates aryl moieties and introduces double bonds in alkyl ones, followed by acid-catalyzed β-scission. This approach significantly improves monomer yields, with the best results constituting a 58–409% increase over conventional maximum monomer yields. The study demonstrates the utility of this method in valorizing various lignins, achieving a 54.0% monomer yield through reductive C–C and C–O cleavage. A techno-economic analysis shows the potential of this method for producing gasoline- and jet-range cycloalkanes and aromatics, while a life-cycle assessment confirms its potential for CO₂-neutral fuel production. The approach is effective for upgrading oligomers obtained by aldehyde-assisted fractionation or RCF from lignocellulosic biomass, as well as various technical lignins, underpinning the broad utility of the method. The study highlights the importance of C–C bond cleavage in lignin valorization and demonstrates the feasibility of a CO₂-neutral lignin biorefinery aimed at fuel production.