In situ growth of carbon nanomaterials on active substance is a very favorable strategy for the preparation of electrode in lithium-ion batteries with excellent electrochemical performance and high stability. Small-sized TiO₂ nanoparticles intercalated into carbon nanosheets (CNS@TiO₂SNP-600) were successfully synthesized via in-situ polymerization-carbonization method, utilizing layered H₂Ti₄O₉ (HTO) as template and benzidine as carbon source. The morphology and size of TiO₂ are greatly influenced by carbonization temperature. The coin cell with the CNS@TiO₂SNP-600 electrode demonstrates a discharge specific capacity of 430.4 mAh×g^-1 at a current density of 0.1 A×g^-1, and the capacity retention rate is 88.1% after 100 cycles; and it also displays a high discharge specific capacity of 101.8 mAh×g^-1 at a high current density of 12.8 A×g^-1. The excellent electrochemical performances can be ascribed to the capacitance effect originated from the intercalated structure of in-situ grown CNS and TiO₂ nanoparticles. We believe this type of materials can be widely used in the lithium-ion batteries and other related green chemical fields.