Lithium intercalation properties of octatitanate synthesized through exfoliation/reassembly process, denoted reassembled-octatitanate, were examined for the first time and compared with those of octatitanate prepared without the exfoliation/reassembly process. Reassembled-octatitanate was prepared by the exfoliation of tetrabutylammonium-intercalated tetratitanate compound and the reassembly of the obtained nanosheets. The electrochemical activity was maintained in the reassembled-octatitanate. The overvoltage of reassembled-octatitanate was smaller than that of a conventional octatitanate. The reversible capacity and energy efficiency of reassembled-octatitanate were 170 (mA h)/g and 91%, respectively, larger than those of a conventional octatitanate. The exfoliation/reassembly process was found to be effective in improving the electrode performance.