Silicon is recognized as the most promising anode material for the next-generation battery. In order to improve the processing and electrochemical performances, a silicon-based anode composite was synthesized using silicon, montmorillonite and carboxymethylcellulose (CMC) as raw materials. The processing parameters, such as particle size and specific surface area, were ameliorated to be consistent with those of commercial lithium-ion battery (LIB) anode materials. As an anode composite, it perfectly matched with high nickel ternary cathode materials and showed excellent electrochemical properties. The discharge capacities were all above 1000 mAh/g and the coulombic efficiency of each step was over 99 % throughout the 50 cycles at 1 C (1100 mA/g). Its superior performances are attributed to the unique layered structure, which buffers the volume expansion and enhances the stability of the solid electrolyte interface (SEI) film on the anodic electrode, suggesting a perspective future in designing high energy density commercial LIBs.