The nanoscale-fabrication of CH3S chains from (CH3S)(2) molecules on Cu(111) was successfully achieved in a controlled step-by-step manner by utilizing the molecular vibration induced by inelastically tunneled electrons. The elementary steps involve: (1) dissociating the S-S bond in an isolated (CH3S)2 molecule to produce two CH3S molecules, (2) bringing a single CH3S molecule close to another to form a dimer by inducing lateral hopping, and (3) elongating the chain from a dimer by repeating the lateral manipulation of CH3S molecules. This study provides a novel method for nanostructuring individual molecules compared with conventional methods utilizing the direct molecule-STM tip interaction. (c) 2006 Elsevier B.V. All rights reserved.