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A unique hybrid nanostructure of ultrathin MoS2 nanosheets on CMK-3 is designed and fabricated as an anode material for lithium-ion batteries. With advantages of the nanosheets-on-channel architecture, the MoS2@CMK-3 electrode is able to deliver a high discharge capacity of 934 mAh g−1 even after 150 cycles at a current density of 400 mA g−1.