Here we report the fabrication of carbon nanotubes (CNTs)/Ni nanocomposite film by electrophoretic deposition (EPD) and subsequent electroless deposition. The present technique requires no pretreatment with expensive Pd species for activation of the surface of CNTs. The EPD bath was modified with NiSO 4 ·6H 2 O to form Ni clusters on the surface of CNTs. As a result, a thin Ni layer (6nm thickness) was fabricated on CNTs, forming a CNT/Ni nanocomposite film with a thickness of 5–10μm. The fabricated CNT/Ni film had nanoporous structure and exhibited electric double layer capacity and catalytic activities for decoloration of methyl orange.