2D nanomaterials, when assembled into an ordered macrostructure, will present many great opportunities, including for Li-ion batteries (LIBs). We report densely-packed vertically-aligned V02(B) nanobelts (NBs)-based forest structure synthesized on edge-oriented graphene (EOG) network Using a EOG/Ni foam as a 3D scaffold, aligned VO2(B) NBs can be further synthesized into a folded 3D forest structure to construct a freestanding electrode for LIBs. Electrochemical studies found that such a freestanding V02(B)/EOG electrode, which combines the unique merits of 2D V02(B) NBs and 2D graphene sheets, has excellent charge-discharge rate performance. A discharge capacity of 178 mAh g-1 at a rate of 59 C and 100 mAh g-1 at 300 C was measured. A good charge-discharge cycling stability under a high current density was also demonstrated. The results indicate V02(B)/EOG forest based freestanding electrode is very promising for developing high-rate LIBs.