In this study, we fabricate an electrode structure, in which a carbon nanotube (CNT) film is coated on the composite of carbon nanotubes (CNTs) and polydimethylsiloxane (PDMS). Electromechanical tests disclose that incorporation of a high density of well-dispersed CNTs (with the aid of UV/O-3 treatment) in the PDMS substrate offers an alternative current path when the CNT film cracked, helping demonstrate much improved electromechanical characteristics. Further analysis using scanning electron microscopy (SEM) combined with the data from the electromechanical tests illuminates some interesting electromechanical features and the failure mechanism of the material. Published by AIP Publishing