Direct plating of electroless Ni-P layers on Al-Ni alloy films formed on glass substrates was performed using magnetron-sputtered deposition and ion beam-assisted deposition methods. Dissolution of Al from the alloy films occurred in the initial stage of the plating process and resulted in enrichment of Ni on the surface. Since Ni acts as a catalyst for the Ni-P deposition reaction, Ni-P deposition occurs on the alloy surface without zincate pretreatment. In the case of an Al-10Ni alloy film, however, Ni clusters dropped from the Al-Ni alloy surface, and Ni-P particles grew in the plating bath, causing dissipation of chemicals in the bath. Such particles also readhered to the surface, resulting in a nonuniform plating layer. A lower concentration of Ni in an alloy such as an Al-3Ni or Al-1Ni alloy resulted in a rather smooth plating surface. In the case of a neutral plating bath containing a low concentration of P, cone structures were formed in the plating layer. Such structures seem to form at the nucleation sites of Ni deposition in the initial stage of the plating process. ©2003 The Electrochemical Society. All rights reserved.