A novel 2D hybrid with MoS(2) nanocrystals strongly coupled on nitrogen-enriched graphene (MoS(2)/NG(g-C(3)N(4))) is realized by mild temperature pyrolysis (550 °C) of a self-assembled precursor (MoS(3)/g-C(3)N(4)-H(+)/GO). With rich active sites, the boosted electronic conductivity and the coupled structure, MoS(2)/NG(g-C(3)N(4)) achieves superior lithium storage performance.