The research has developed a novel method of Nanopillar array through the combination of integrating self-assembly nanosphere lithography and photo-assisted electrochemical etching technique. The self-assembly nanosphere lithography technique can be used to define nano-pattern array by the novel coating method. The novel coating method of nanosphere can regular arrange nanosphere in some region of whole 1 cm2 wafer. In experiment of photo-assisted electrochemical etching, surfactant can reduce contact angle of electrolyte and obtain high aspect ratio of nanohole easily. The highest aspect ratio of nanohole is 68:1. We have finished the novel fabrication process of nanopillar array without expensive equipments. Nanopillar can regular arranged, which dimensions is 70 nm~50 nm wide and 1000 nm tall (aspect ratio, 14~20:1). Keywords: nanopillar, nanosphere, electrochemical etching, self-assembly.