A nonwoven nanofiber fabric with paper-like qualities composed of Si nanoparticles and carbon as binder-free anode electrode is reported. The nanofiber fabrics are prepared by convenient electrospinning technique, in which, the Si nanoparticles are uniformly confined in the carbon nanofibers. The high strength and flexibility of the nanofiber fabrics are beneficial for alleviating the structural deformation and facilitating ion transports throughout the whole composited electrodes. Due to the absence of binder, the less weight, higher energy density, and excellent electrical conductivity anodes can be attained. These traits make the composited nanofiber fabrics excellent used as a binder-free, mechanically flexible, high energy storage anode material in the next generation of rechargeable lithium ions batteries.