Electrodes with novel architectures may enable the construction of high power density batteries with ultrafast charge/discharge performances, which are fundamental for todays power tools, medical devices and transportation systems. Hereby, we demonstrate the application of vertically arranged multilayered-graphene, namely carbon nanowalls (CNW), as a potential high power anode to be used in Li-ion secondary batteries. CNWs are deposited onto Cu foils using microwave plasma enhanced chemical vapor deposition (MPE-CVD) technique. MPE-CVD is a simple and rapid technique, which is effectively proven to produce self-standing layered anodes by single step processing. The direct deposition over Cu avoids the addition of foreign ingredients such as binders and conductive agents. This opens up the possibility to reduce the number of processing steps and processing time, which are key aspects when upscaling is sought. The superior cycling behaviour of the newly elaborated CNWs is demonstrated in lab-scale Li-metal and Li-ion cells (LiFePO4 cathode) capable of very stable and prolonged reversible cycling with excellent durability (>1000 cycles), good specific capacity and capacity retention when subjected to ultrafast current regimes.