Currently, common two-dimensional (2D) carbon materials composited with Si-based materials as anode for lithium-ion batteries exhibit excellent electrochemical properties. In this study, we describe the one-step synthesis of amino-functionalized mesoporous silica (SiO2) nanospheres through self-assembly. Morphology modulation and amino group grafting were performed simultaneously without secondary modification. Using tartaric acid and melamine as dual carbon sources, the 2D lamellar structure was constructed using the dehydration condensation reaction, with the mesoporous SiO2 nanospheres uniformly intercalated within the carbon sheets. The composites were securely bonded by chemical bonding, effectively addressing the issue of structural collapse often encountered in silica–carbon composites. Ultimately, the lamellar SiO2@NC composite exhibited stable capacity of 539.5 mAh g−1 after 500 cycles at 1 A g−1. This strategy is simple and effective, compared to the complex processes typically associated with 2D carbon materials synthesis, and can be potentially extended to applications in catalysis, adsorption, and separation within diverse fields.