In this work, homogeneous Ni_0.33Co_0.67Se hollow nanoprisms were synthesized successfully in virtue of Kirkendall effect. It is the first time for bimetallic Ni-Co compounds Ni_0.33Co_0.67Se to be used in lithium-ion batteries (LIBs). Impressively, the Ni_0.33Co_0.67Se hollow nanoprisms show superior specific capacity (1, 575 mAh/g at the current density of 100 mA/g) and outstanding rate performance (850 mAh/g at 2, 000 mA/g) as anode material for LIBs. This work proves the potential of bimetallic chalcogenide compounds as high performance anode materials for LIBs.