Carbon　composite　materials　consisting　of　onion-like　carbons　(OLCs)　and　vertically　aligned　graphene　nanoribbons　(VA-GNRs)　have　been　efficiently　prepared　by　an　atomic　hydrogen　treatment.　SiC　is　employed　as　the　seed　for　growing　nanodiamonds,　which　serve　as　precursors　and　convert　into　OLCs.　The　obtained　OLCs　are　quasi-spherical　in　shape　with　closed　concentric　graphite　shells　without　a　core.　The　original　vertical　structural　integrity　and　alignment　of　VA-GNRs　is　well　preserved,　and　the　OLCs　remain　highly　porous.　The　electrochemical　measurements　show　that　the　OLC-GNRs　composite　exhibits　higher　capacitive　properties　than　the　original　vertically　aligned　single　walled　carbon　nanotubes　(VA-SWCNTs)　carpet　and　VA-GNRs.　This　composite　nanostructure　demonstrates　a　high　performance　in　maximum　specific　energy　(36.4　Wh　kg(-1)),　specific　power　(270.2　kW　kg(-1)),　and　cycle　stability　(no　drop　after　10　000　cycles).　The　superior　electrochemical　performance　of　the　OLCs-GNRs　composite　electrode　can　be　attributed　to　the　higher　specific　surface　area　of　the　additional　porous　OLCs,　and　the　vertical　alignment　of　the　conductive　paths　of　VA-GNRs.　All　demonstrate　that　atomic　hydrogen　treatment　is　an　attractive　approach　to　fabricate　electrodes　for　supercapacitors　with　high　power　and　energy　density.