Two-dimensional (2D) nanostructure patterns have extensive applications in photonic devices, nanoelectronics, electrochemical devices, biosensors, catalysts and high-density magnetic recording devices. It remains a challenge to develop low-cost, high-throughput, high-resolution techniques for the fabrication of large-area (wafer-scale) 2D nanostructure array patterns with controlled feature size, shape and pitch. The present work has demonstrated a low-cost, high-throughput, high-resolution approach for the fabrication of large-area, high-quality nanostructure array patterns by nanosphere lithography combined with electroplating. The gold hemisphere array pattern obtained is capable of functioning as a nanoelectrode array (NEA) in which the gold hemispheres act as individual electrodes that are separated with an insulating polypyrrole (PPY) film. Cyclic voltammetry measurement has shown a sigmoid-shaped voltammogram, which is characteristic of electrochemical characteristics of a nanoelectrode array. NEAs are expected to find extensive applications in fundamental electrochemistry studies and electrochemical devices.