The long-term stability of energy-storage devices for green energy has received significant attention. Lithium-ion batteries (LIBs) based on materials such as metal oxides, Si, Sb, and Sn have shown superior energy density and stability owing to their intrinsic properties and the support of conductive carbon, graphene, or graphene oxides. Abnormal capacities have been recorded for some transition metal oxides, such as NiO, Fe2O3, and MnO/Mn3O4. Recently, the restructuring of NiO into LiNiO2 anode materials has yielded an ultrastable anode for LIBs. Herein, the effect of the thin film thickness on the restructuring of the NiO anode was investigated. Different electrode thicknesses required different numbers of cycles for restructuring, resulting in significant changes in the reconstituted cells. NiO thicknesses greater than 39 μm reduced the capacity to 570 mAh g−1. The results revealed the limitation of the layered thickness owing to the low diffusion efficiency of Li ions in the thick layers, resulting in non-uniformity of the restructured LiNiO2. The NiO anode with a thickness of approximately 20 μm required only 220 cycles to be restructured at 0.5 A g−1, while maintaining a high-rate performance for over 500 cycles at 1.0 A g−1, and a high capacity of 1000 mAh g−1.