Herein we present the preparation of novel multifunctional metallic nickel/oxide (Ni/NiO) hybrid nanomembranes with rough and undulating surface morphologies, by a physical deposition method combined with chemical etching and thermal oxidation. Benefiting from the advantages of intrinsic architecture and electrochemical catalysis of metallic nickel, the anodes can be discharged and charged at an ultrahigh rate of ~115C (1C=718mAg−1) if only the mass of NiO is taken into calculation or 60C if the total mass of Ni/NiO nanomembranes is considered. To our knowledge, this is the best reported rate performance for NiO-based anodes in Li-ion batteries to date. Furthermore, excellent cycling stability is also demonstrated.