Lignin,　characterized　by　its　amorphous,　heavily　polymerized　structure,　is　a　primary　natural　source　of　aromatic　compounds,　yet　its　complex　constitution　poses　considerable　challenges　in　its　transformation　and　utilization.　Therefore,　the　selective　cleavage　of　C-C　bonds　represents　a　critical　and　challenging　step　in　lignin　degradation,　essential　for　the　production　of　high-value　aromatic　compounds.　In　this　study,　we　report　a　simple　electrocatalytic　approach　for　lignin　valorization　via　C-C　bond　cleavage　by　developing　a　nonmetallic　electrocatalyst　of　carbon-based　materials.　It　is　found　that　the　hydrophilicity　and　hydrophobicity　of　the　electrocatalyst　have　a　significant　effect　on　the　degradation　process.　Under　mild　conditions,　the　hydrophilic　carbon　paper　exhibits　100%　substrate　conversion,　yielding　97%　benzaldehyde　and　96%　quinone　with　ionic　liquid　electrolytes.　The　mechanism　study　shows　that　the　carbon　catalyst　with　higher　surface　defects　favors　electron　transfer　in　the　oxidative　cleavage　process　of　C-C　bonds.　These　results　signify　a　substantial　advancement　in　lignin　degradation,　offering　an　environmentally　friendly,　metal-free　electrochemical　route.　©　2024　The　Authors.　Co-published　by　Zhejiang　University　and　American　Chemical　Society.