The nanocomposites of MoS2 nanosheets and microporous nitrogen-doped carbon dodecahedron (MNCD) are prepared through the pyrolysis of metal-organic framework (MOF) and subsequent growth of MoS2. The porous and active surface of MNCDs enables uniform growth of ultrathin MoS2 nanosheets. When the MNCD@MoS2 composite is used as the anode material of Li-ion batteries, a reversible capacity of 915 mAh g−1 can be obtained even at the extremely high current density of 10 A g−1. The ultrafast charge/discharge ability of MNCD@MoS2 can be attributed to its unique core-shell structure with the inner MNCDs serving as the reservoir of Li-ions and transport media of electrons.