Natural　nitrogen-heterocycles　biomolecules　have　been　widely　used　in　the　construction　of　supramolecular　self-assemblies　due　to　their　abundant　resources　and　multiple　interaction　sites,　such　as　hydrogen　bonding,　π-π　stacking,　van　der　Waals　forces.　Herein,　we　propose　a　quite　innovative　strategy　to　produce　two-dimensional　(2D)　carbon　materials　by　direct　pyrolysis　of　various　nucleobases　(e.g.　guanine,　adenine,　uracil,　cytosine　xanthine,　and　hypoxanthine).　These　nucleobases　can　pre-organize　a　planar　network　structure　through　hydrogen　bonding　interaction.　The　multiple　hydrogen-bonding　can　be　stable　at　relatively　high　temperature,　which　limits　C–C　or　C-N　cleavage　and　formation　in　a　2D　space.　These　2D　carbons　show　desirable　features　with　highly　sp2-conjugation,　tunable　heteroatom　contents,　and　ultrathin　thickness,　without　the　need　of　any　template　or　additional　purification.　Meanwhile,　differences　in　internal　structure　allow　easy　control　of　the　morphology　of　2D　carbons,　porosity　and　surface　chemical　functionality　at　the　molecular　level.　Moreover,　the　as-synthesized　2D　carbons　display　very　promising　electrocatalytic　ORR　performance　and　catalytic　performance　for　selective　oxidization　of　ethylbenzene.　Given　the　diversity　in　the　structure　of　the　nucleobase　moiety,　they　represent　ideal　building　blocks　for　the　catalyst-free　and　metal-free　formation　of　2D　carbon　architectures.　©　2022　Elsevier　B.V.