performance, and rate capability of current LIBs are not suffi cient to fully meet the demands for other emerging applications, such as electric vehicles and green energy grids. [4][5][6][7] Possible breakthroughs in LIBs with superior electrochemical performance depend in large part on the development of new electrochemically active electrode materials. Thus, the exploitation of different anode materials with high capacity is of strong interest. Among high-capacity anode materials, metal oxides are particularly attractive due to their high theoretical capacity, low toxicity, and low cost. [8][9][10] Nevertheless, metal oxide anode materials for LIBs usually suffer from rapid capacity decay during cycling and poor rate performance due to their intrinsically low conductivity, large volume expansion during lithiation, and the formation of a thick solid electrolyte interface (SEI). [ 8,11 ] To circumvent these obstacles, several strategies have been developed to engineer new metal oxide materials with special nanostructures as suitable matrices for enhancing LIBs. [ 8,12 ] Although the above problems can be alleviated by using these approaches, the challenge remains to achieve metal oxide anodes with superior capacity and stability for applications in electric vehicles. Recent studies suggest a promising trend in the formation of anode materials with superior performance based on the combination of nanostructure and nanocomposite strategies. [ 13,14 ] In this respect, graphene was used to fabricate hybrid nanomaterials with improved electrochemical performance due to its superior electric conductivity, good mechanical fl exibility, and high chemical stability. [ 15,16 ] Although some impressive improvements were observed, some disadvantages for lithium storage remain with these hybrids, including undesired aggregation during the cycle processes. [ 17 ] Further design and fabrication of these nanocomposites as well as nanostructures are needed to achieve metal oxide-based anodes with superior performance.Various natural materials with specifi c nanostructures have attractive properties as synthetic templates in nanotechnology to regulate the synthesis of metal oxides with desired nanostructures. [ 18 ] These materials can also stabilize nanosized metal oxide materials as matrices to restrain aggregation and then be transformed into amorphous carbon by annealing to further improve electrochemical stability of the products. Silk fi broin (SF), a high molecular weight amphiphilic protein polymer, has been successfully used to prepare different nanomaterials when used as a template.