Here, we report the synthesis of aligned carbon nanotube (CNT) bundles with adjustable arrays by a non-lithographic and low-cost strategy. A polystyrene/ferrocene patterns on silicon (Si) substrate was prepared through controlled mesoscopic dewetting of dilute polystyrene/ferrocene solution. A variety of regular patterns, including ladder, stripe and scale, were synthesized simply by changing the solution concentration. Ultraviolet (UV) irradiation effectively cross-linked polymer skeleton and made it suitable for structure-directing agent. In the sequent pyrolysis, polystyrene skeleton was decomposed and ferrocene was converted into the skeleton of inorganic patterns simultaneously. Aligned CNT bundles guided by the catalytically functionalized inorganic patterns were initiated to grow. This methodology opens up a new avenue for fabricating CNT arrays in a simple and controllable manner. Crown Copyright (c) 2012 Published by Elsevier Ltd. All rights reserved.