The　applications　of　carbon-based　supercapacitors　have　been　limited　by　their　low　energy　storage　density　owing　to　their　limited　active　storage　sites.　To　overcome　this　limitation,　amine-enriched　porous　carbon　electrodes　have　been　fabricated　by　the　electrostatic　fusion　of　amine-functionalized　single-crystalline　graphene　quantum　dots　(GQDs)　within　conductive,　vertically　ordered　TiO2　nanotube　arrays　as　the　collectors.　The　carbon　films　deliver　ultrahigh　specific　capacitance　(400-595　F　g(-1))　even　beyond　the　theoretical　upper　limit　of　single-layer　graphene　by　inducing　a　high　concentration　of　active　amine　moieties　at　edge.　Symmetrical　GQD　supercapacitors　in　H2SO4　electrolyte　offer　energy　density　up　to　21.8　Wh　kg(-1)　and　retain　90%　of　the　initial　capacitance　after　10000　cyclic　voltammetry　tests.　The　results　show　that　amine-enriched　GQDs　can　function　as　a　new　kind　of　highly　active,　solution-processable,　and　low-cost　pseudocapacitive　materials　applicable　to　high-performance　supercapacitors.　(C)　2016　Elsevier　Ltd.　All　rights　reserved.