Mo2C　nanocrystals　(NCs)　anchored　on　vertically　aligned　graphene　nanoribbons　(VA-GNR)　as　hybrid　nanoelectrocatalysts　(Mo2C-GNR)　are　synthesized　through　the　direct　carbonization　of　metallic　Mo　with　atomic　H　treatment.　The　growth　mechanism　of　Mo2C　NCs　with　atomic　H　treatment　is　discussed.　The　Mo2C-GNR　hybrid　exhibits　highly　active　and　durable　electrocatalytic　performance　for　the　hydrogen-evolution　reaction　(HER)　and　oxygen-reduction　reaction　(ORR).　For　HER,　in　an　acidic　solution　the　Mo2C-GNR　has　an　onset　potential　of　39　mV　and　a　Tafel　slope　of　65　mV　dec(-1),　and　in　a　basic　solution　Mo2C-GNR　has　an　onset　potential　of　53　mV,　and　Tafel　slope　of　54　mV　dec(-1).　It　is　stable　in　both　acidic　and　basic　media.　Mo2C-GNR　is　a　high-activity　ORR　catalyst　with　a　high　peak　current　density　of　2.01　mA　cm(-2),　an　onset　potential　of　0.93　V　that　is　more　positive　vs　reversible　hydrogen　electrode　(RHE),　a　high　electron　transfer　number　n　(similar　to　3.90),　and　long-term　stability.