A layered tin-aminoclay structure of high specific surface area and offering great mechanical resistance to stretching is used as an improved anode for lithium-ion battery application. The active nanoparticles (Sn/SnO/SnO2 nanoparticles) are evolved by a heat-treatment process through direct conversion of Sn species within tin-aminoclay structure. Besides, this heat treatment process facilitates removal of oxygen functionalities and homogenization of the tin-aminoclay surface, and also provides great synergistic effects, all leading to improved theoretical specific capacity and electrochemical performance in lithium-ion battery applications. Thus, tin-aminoclay heat-treated at 500 °C under the argon condition is considered to be a most promising candidate anode material one that can deliver a highest initial discharge capacity value of 1,400 mAh g−1, good stability after 95 repeated cycles, and a high reversible capacity of about 500 mAh g−1 at a current density of 100 mA g−1.