Y. Zhang, X.-B. Zhang, and co-workers report on page 4345 an electrostatic-induced spread-growth method to homogeneously coat CoO on graphene. Binder-free electrode with excellent structural stability can then be easily prepared by layer-by-layer stacking. As an anode for Li-ion batteries, the asprepared electrode exhibits a high rate capability and excellent cycle stability up to 5000 cycles. This opens up a promising strategy to develop high-performance anodes for next-generation LIBs.