Pd　nanoparticles　(similar　to　2.1　nm)　supported　on　biomolecule-derived　graphene-like　carbons　have　been　studied　as　highly　active　and　stable　catalysts　for　the　selective　hydrogenation　of　quinolines.　A　novel　strategy　is　developed　by　pyrolysis　of　guanine　with　H2SO4,　yielding　heteroatom-doped　(N/O,　N/O/S)　and　minimally　layered　carbon　nanosheets　with　large　accessible　areas,　which　can　facilitate　mass　transfer　and　stabilize　Pd　nanoparticles.　XPS　results　indicate　that　the　intensity　ratio　of　Pd-0/Pd2+　increases　with　N/S　codoping　in　graphene-like　carbons,　suggesting　a　significant　correlation　between　support　properties　and　electronic　structure　of　Pd　species.　N/O/S-codoped　Pd@GS1000　shows　substantially　enhanced　activity　for　quinoline　hydrogenation　reactions,　with　almost　＞99%　conversion　and　＞99%　selectivity　to　1,2,3,4-tetrahydroquinoline　under　mild　catalytic　conditions,　superior　to　Pd@G1000　(without　sulfur　doping)　and　the　reference　Pd/OCNT　catalyst.　Further　investigation　indicates　that　sulfur　containing　carbon　nanosheets　strongly　interact　with　metal　supports,　and　thus　metallic　Pd　can　be　regarded　as　an　active　center　for　hydrogenation　reactions.　This　work　may　provide　a　framework　for　the　development　of　promising　applications　of　supported　catalysts　based　on　ultrathin　carbon　nanosheets　in　fine　chemical　production.