Manganese oxide nanoflower/carbon nanotube array (CNTA) composite electrodes with hierarchical porous structure, large surface area, and superior conductivity was controllable prepared by combining electrodeposition technique and a vertically aligned CNTA framework. This binder-free manganese oxide/CNTA electrode presents excellent rate capability (50.8% capacity retention at 77 A/g), high capacitance (199 F/g and 305 F/cm 3 ), and long cycle life (3% capacity loss after 20 000 charge/discharge cycles), with strong promise for high-rate electrochemical capacitive energy storage applications.In development of energy storage devices, nanostructured electrode materials have attracted great interest, as they show not only higher capacities but also better rates than traditional materials. 1-6 Nanostructured electrode materials are key components in the advancement of future energy technologies; thus, strategies for preparing high-performance nanomaterials are required. 5 However, direct synthesis of complex nanostructures still remains a challenge in areas of materials science. 7,8 Nowadays, much research on electrochemical capacitors (ECs) is aimed at increasing power and energy densities as well as lowering fabrication costs while using environmentally friendly materials. Specifically, it was found that RuO 2 exhibits prominent capacitive properties as ECs electrode materials; 9 however, its high cost excludes it from wide application. Relatively low cost materials such as MnO x and NiO x can also be used as electrode materials, but their poor rate capability need to be enhanced. 10,11 Manganese oxides (MO) have been thoroughly investigated because of their importance in industrial applications, such as catalysis and energy storage. [12][13][14][15][16] Over the years various nanostructured manganese oxides, including dendritic clusters, nanocrystals with different shapes, nanowires, nanotubes, nanobelts, and nanoflowers, have been synthesized. [17][18][19][20][21][22][23][24] In order to greatly increase electrochemical performance of manganese oxides, a hierarchical porous structure 25 with high electronic conductivity 26 must be considered. Nevertheless, up to now, no method has been reported to fabricate hierarchical porous and binder-free manganese oxide composite electrodes with superior electronic conductive paths. In this paper, we realized this goal by a combination of a carbon nanotube array (CNTA) framework and an electrodeposition technique to fabricate a composite structure, that is, well-dispersed manganese oxide nanoflowers on a vertically aligned CNTA. CNTA is excellent for electrodepositing transition metal oxides because of its regular pore structure, high surface area, homogeneous property (binderfree), and excellent conductivity. [27][28][29][30] The experimental results show that the manganese oxide/CNTA composite electrode exhibits superior rate performance (50.8% capacitance retention at 77 A/g) in an EC, thus, making it very promising for high-rate electrochemical capacitive energy ...