Nanostructured NiCo₂O₄ is directly grown on the surface of three-dimensional graphene-coated nickel foam (3D-GNF) by a facile electrodeposition technique and subsequent annealing. The resulting NiCo₂O₄ possesses a distinct flower or sheet morphology tuned by potential or current variation electrodeposition, which is used as a binder-free lithium ion battery anode for the first time. Both samples exhibit high lithium storage capacity profiting from unique binder-free electrode structures. The flower-type NiCo₂O₄ demonstrates high reversible discharge capacity (1459 mAh g^–1 at 200 mA g^–1) and excellent cyclability with around 71% retention of the reversible capacity after 60 cycles, which are superior to sheet-type NiCo₂O₄. Such superb performance can be attributed to high volume utilization efficiency with unique morphological character, a well-preserved connection of active materials to the current collector, a short lithium ion diffusion path, and fast electrolyte transfer in binder-free NiCo₂O₄-coated 3D graphene structure. The simple preparation process and easily controllable morphology make binder-free NiCo₂O₄/3D-GNF hybrid a potential material for commercial application.