Metal oxide/carbonaceous nanomaterials are promising candidates for energy-storage applications. However, inhomogeneous mass and charge transfer across the electrode/electrolyte interface due to unstable metal oxide/carbonaceous nanomaterial synthesis limit their performance in supercapacitors. Here, it is shown that the above problems can be mitigated through stable low-current electrodeposition of MnO2 on superaligned electrospun carbon nanofibers (ECNFs). The key to this approach is coupling a self-designed four steel poles collector for aligned ECNFs and a constant low-current (40 mu A) electrodeposition technique to form a uniform Na+-induced alpha-MnO2 film which proceeds by a time-dependent growth mechanism involving cluster-"kebab" structures and ending with a compact, uniform MnO2 film for high-performance energy storage.