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With the ever-increasing world population, the energy produced from green, environmentally friendly approaches is in high demand. In this work, we proposed a green and cost-effective strategy for synthesizing a porous carbon electrode decorated with alumina oxide (Al₂O₃) from cherry blossom leaves using the pyrolysis method followed by a sol-gel method. An Al₂O₃-coating nano-layer (4–6 nm) is formed on the porous carbon during the composition fabrication, which further adversely affects battery performance. The development of a simple rich-shell-structured C@Al₂O₃ nanocomposite anode is expected to achieve stable electrochemical performances as lithium storage. A significant contributing factor to enhanced performance is the structure of the rich-shell material, which greatly enhances conductivity and stabilizes the solid–electrolyte interface (SEI) film. In the battery test assembled with composite C@Al₂O₃ electrode, the specific capacity is 516.1 mAh g⁻¹ at a current density of 0.1 A g⁻¹ after 200 cycles. The average discharge capacity of carbon is 290 mAh g⁻¹ at a current density of 1.0 A g⁻¹. The present study proposes bioinspired porous carbon electrode materials for improving the performance of next-generation lithium-ion batteries.