ABSTRACT In this paper we report a novel architecture of three-dimension (3D) carbon framework to encapsulate tetrahedron ZnO nanocrystals that serves as an anode material for lithium-ion batteries (LIBs). The ZnO@C composites are prepared via a simple internal-reflux method combined with subsequent calcination in argon. The amorphous carbon is formed on the surface of the ZnO crystals by in situ carbonization of the surfactant, which leads to a strong connection between the carbon framework and the active materials and guarantees faster charge transfer on the electrode. The ZnO crystal calcined at 500°C (ZnO@C-5) possesses regular tetrahedron shape with a side length of 150-200nm and all of them are uniformly anchored among the network of amorphous carbon. The developed ZnO@C structures not only improve the electronic conductivity of the electrode, but they also offer a larger volume expansion of ZnO during cycling. As a result, the ZnO@C-5 demonstrates a higher reversible capacity, ultralong cycle life and better rate capability than that of the ZnO@C-7 and pure ZnO crystals. After 300 cycles, the ZnO@C-5 demonstrates a high capacity of 518mAhg−1 at a current density of 110.7mAg−1. Moreover, this simple approach prepared the 3D composites architecture could shed light on the design and synthesis of other transition metal oxides for energy storage.