This article reports a novel method for breaking carbon–carbon (C–C) bonds in lignin, which are challenging to cleave without pre-functionalization. The approach involves using a Pt/H-MOR catalyst to selectively cleave various C–C linkages (5–5′, β–1′, β–5′, and β–β′) under mild conditions (≤310 °C). This method significantly increases monomer yields compared to conventional strategies that primarily target C–O bonds. The catalyst's bifunctional nature, combining Pt hydrogenation and Bronsted acid sites, allows for the selective cleavage of aryl–aryl, aryl–alkyl, and alkyl–alkyl bonds. The effectiveness of this method is demonstrated through the successful depolymerization of model lignin dimer and various technical lignins, achieving yields up to 58–409% higher than the maximum monomer yield obtainable through conventional methods. The techno-economic analysis and life-cycle assessment of a biorefinery based on this approach show its potential for producing gasoline- and jet-range cycloalkanes and aromatics, with a promise of CO2-neutral fuel production.This article reports a novel method for breaking carbon–carbon (C–C) bonds in lignin, which are challenging to cleave without pre-functionalization. The approach involves using a Pt/H-MOR catalyst to selectively cleave various C–C linkages (5–5′, β–1′, β–5′, and β–β′) under mild conditions (≤310 °C). This method significantly increases monomer yields compared to conventional strategies that primarily target C–O bonds. The catalyst's bifunctional nature, combining Pt hydrogenation and Bronsted acid sites, allows for the selective cleavage of aryl–aryl, aryl–alkyl, and alkyl–alkyl bonds. The effectiveness of this method is demonstrated through the successful depolymerization of model lignin dimer and various technical lignins, achieving yields up to 58–409% higher than the maximum monomer yield obtainable through conventional methods. The techno-economic analysis and life-cycle assessment of a biorefinery based on this approach show its potential for producing gasoline- and jet-range cycloalkanes and aromatics, with a promise of CO2-neutral fuel production.