Protein has abundant and exquisite multidimensional structures and numerous functional groups that can bind metal ions. Taking protein as a template can effectively promote the synthesis of metal oxide nanomaterials and form multidimensional network structures, which has great prospects in preparing high-performance lithium-ion battery (LIB) anode. However, these templates only act as carbon skeletons to support electrode materials. The biodiversity of proteins in precise regulation is not fully realized, limiting the application potential of protein templates. In this work, we selected biomineralized protein BSA as the template for the electrode materials synthesis, successfully regulated the nanocrystal and microstructure, and obtained a highquality anode material with nanonetwork and ultrathin nanolayer structure. The nanocrystals of synthesized anode materials showed good uniformity and monodispersity, achieved the heteroatom doping, such as N and S elements, and in situ carbon coating. The carbon nanolayer structure formed by BSA protein improved the capacitance and stability of electrode materials, revealing a good application value for the LIB anode. This research can give us a further understanding and expand the idea of protein templates in the preparation of high-performance energy storage nanomaterials.