A nonwoven fabric with paperlike qualities composed of silicon nanowires is reported. The nanowires, made by the super-critical-fluid-liquid-solid process, are crystalline, range in diameter from 10 to 50 nm with an average length of > 100 mu m, and are coated with a thin chemisorbed polyphenylsilane shell. About 90% of the nanowire fabric volume is void space. Thermal annealing of the nanowire fabric in a reducing environment converts the polyphenylsilane coating to a carbonaceous layer that significantly increases the electrical conductivity of the material. This makes the nanowire fabric useful as a self-supporting, mechanically flexible, high-energy-storage anode material in a lithium ion battery. Anode capacities of more than 800 mA h g(-1) were achieved without the addition of conductive carbon or binder.