Hierarchically designed SiOx/SiOy rolled-up bilayer nanomembranes are used as anodes for lithium-ion batteries. The functionalities of the SiO(x,y) layers can be engineered by simply controlling the oxygen content, resulting in anodes that exhibit a reversible capacity of about 1300 mA h g(-1) with an excellent stability of over 100 cycles, as well as a good rate capability.