The coaxial MnO2/CNTs nanocomposite freestanding membrane is prepared via a simple two-step process, including that CNTs are grown on the surface of stainless steel mesh by chemical vapor deposition and then MnO2 is coated onto the surface of CNTs using electrodeposition. Scanning electron microscopy and transmission electron microscopy demonstrate that MnO2 nanoflakes are uniformly deposited on the surface of CNTs to form the coaxial MnO2/CNTs nanocomposites freestanding membrane. The thickness of MnO2 shell is in range of 25–50nm. Electrochemical characterizations shows that the initial discharge capacity of MnO2/CNTs nanocomposites freestanding membrane is as high as 2062mAhg−1 based on the total mass of MnO2/CNTs nanocomposites, and its capacity retention is 80% after 260cycles compared with the second cycle. The result suggests that the as-prepared coaxial MnO2/CNTs nanocomposite freestanding membrane anode indicates excellent cycle stability and good rate capability. Moreover, it can be prepared on a large scale and suitable for industrial production due to its simple and low-cost prepared process.