With the development of the portable and wearable electronic devices, there has been an increasing demand for flexible, lightweight, high performance, and environmentally friendly energy storage/conversion systems.[1] Carbon nanotubes (CNTs) have been recognized as one of the most attractive framework materials for high-performance supercapacitors, due to high electrical and mechanical properties, and excellent chemical stability. And manganese oxides (MnO2) is one of the foremost pseudocapacitance materials. Once we want to combine them together to obtain a high performance electrode, the deposited MnO2 usually forms into bulky clusters on the CNTs because of only a few surficial defects on the CNTs. These bulky clusters often lead to a low utilization efficiency of pseudocapacitance materials.[2]