A sponge-like ε-MnO2 nanostructure was synthesized by direct growth of ε-MnO2 on Ni foam through a facile electrodeposition route. When applied as a self-supporting, binder-free cathode material for rechargeable nonaqueous lithium-oxygen batteries, the ε-MnO2/Ni electrode exhibits considerable high-rate capability (discharge capacity of ∼6300 mA h g(-1) at a current density of 500 mA g(-1)) and enhanced cyclability (exceeding 120 cycles) without controlling the discharge depth. The superior performance is proposed to be associated with the 3D nanoporous structures and abundant oxygen defects as well as the absence of side reactions related to carbon-based conductive additives and binders.