Ni-coated ZnO was prepared by electroless nickel plating as an anode material for lithium-ion batteries. The microstructure of the Ni-coated ZnO was characterized by means of X-ray diffraction, transmission electron microscopy, and energy dispersive X-ray spectroscopy. The electrochemical properties of the anodes were measured by galvanostatic charge-discharge tests and electrochemical impedance spectroscopy. The results show that the Ni-coated ZnO delivered a higher reversible discharge capacity <mml:math display="inline"><mml:mrow><mml:mo>(</mml:mo><mml:mn>490</mml:mn><mml:mspace width="0.3em"></mml:mspace><mml:mi>mAh</mml:mi><mml:mspace width="0.3em"></mml:mspace><mml:msup><mml:mi mathvariant="normal">g</mml:mi><mml:mrow><mml:mo>−</mml:mo><mml:mn>1</mml:mn></mml:mrow></mml:msup><mml:mo>)</mml:mo></mml:mrow></mml:math>(490mAhg−1) than the raw ZnO <mml:math display="inline"><mml:mrow><mml:mo>(</mml:mo><mml:mn>130</mml:mn><mml:mspace width="0.3em"></mml:mspace><mml:mi>mAh</mml:mi><mml:mspace width="0.3em"></mml:mspace><mml:msup><mml:mi mathvariant="normal">g</mml:mi><mml:mrow><mml:mo>−</mml:mo><mml:mn>1</mml:mn></mml:mrow></mml:msup><mml:mo>)</mml:mo></mml:mrow></mml:math>(130mAhg−1) , exhibited good cyclability, and the initial coulombic efficiency of the ZnO was significantly improved after coating (from 49.5% to 75%). The presence of the nickel membrane plays three important roles in the improvement of initial coulombic efficiency and the cycling performance of ZnO. First, nickel as a conductor can improve the high rate properties of ZnO. Second, nickel acts as a buffer to alleviate the stress during cycling. Third, nickel also has the catalytic activity to facilitate <mml:math display="inline"><mml:mrow><mml:msub><mml:mi mathvariant="normal">Li</mml:mi><mml:mrow><mml:mn>2</mml:mn></mml:mrow></mml:msub><mml:mi mathvariant="normal">O</mml:mi></mml:mrow></mml:math>Li2O decomposition.