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Silicon（Si） has become one of the hot spots in the research of anode materials in lithium-ion batteries (LIBs) for its highest lithium intercalation capacity among known elements. However, the large volume expansion (~300%) of Si due to the lithium intercalation restricts its application in LIBs. Nano-crystalized is an effective solution to resolve the volume expansion. Nano-Si was prepared by high-energy electron beam and mechanical grinding method, using metallurgical Si. According to scanning electron microscopy (SEM) observation, the molten Si was deposited into Si nanofibers with a linear diameter of about 40nm after evaporation under the action of high-energy electron beam, and then gathered into Si nanobundles, and the size distribution of nano-Si particles after mechanical grinding is uniform. The results of electrochemical tests show that the first reversible capacity is 1292.4mAh/g, and the charge transfer impedance fitting value is 51.36Ω, under the condition of the nano-Si purity reaches more than 99.96% and the discharge density is 100mAh/g. The experimental results indicates that this method can be applied to controllable and large-scale prepare nano-Si, and gives a guidance that how to scalable use Si in LIBs industry.