Nickel and other metal nanoparticles are known to be active as catalysts in the synthesis of carbon nanofibers. In this paper we investigate how dewetting and break-up of nickel thin films depends on film thickness, film-substrate interaction and pretreatment conditions. This is evaluated for films evaporated on oxidized silicon and fused silica substrates with or without tantalum coating, which were subsequently exposed to different pretreatment atmospheres (vacuum, nitrogen, air and hydrogen; 1 h, 650 degrees C). Atomic force microscopy, scanning electron microscopy and energy dispersive X-ray analysis were used to characterize the films. Pretreated Ni films were subjected to a thermal catalytic chemical vapor deposition procedure with brief ethylene exposures (0.5-3 min, 635 degrees C). It was found that only on the spherical nanoparticles originating from a hydrogen pretreatment of a Ni film with Ta adhesion layer, homogeneously distributed, randomly-oriented, well-attached, and semi-crystalline carbon nanofibers be synthesized. (C) 2013 Elsevier B.V. All rights reserved.