In this work, an innovative 3D-frame structure ultrathin NiO nanosheets/carbon nanotubes (CNTs) composite as anode for lithium-ion batteries (LIBs) was successfully fabricated via a facile, effective strategy. Our 3D-frame structure NiO@CNTscompositebasedanodeforLIBsalsoshowsultrahighcapacity (*), rate, cycle and Coulombic efficiency performance for the ultrafast charge slow discharge. When using 100mAg−1 to charge and 2000mAg−1 to discharge (half-cell), the charge and discharge capacity of the NiO@CNTs composites reached 763 and 1000mAhg−1 at the first cycle, respectively. From the 2nd cycle the Coulombic efficiency is higher than 95%, and after 100 cycles the capacity maintained 122.7% based on capacity of the second cycle.