Electroless plating of nickel (or copper) was carried out on glass (or silicon) substrates that were previously surface modified by using plasma-polymerization and grafting processes, and then activated by immersion in a simple acidic PdCl(2) solution. Three pretreatments based on the deposition of plasma-polymerized thin films (PACVD process) on O(2) plasma-cleaned substrates were investigated. They include film deposition of (1) amorphous hydrogenated carbon (a-C:H) grown from CH(4), whose surface is subsequently plasma-functionalized in NH(3) or N(2); (2) amorphous hydrogenated carbon nitride (a-CN(x):H) grown from CH(4)/NH(3) or CH(4)=N(2) mixtures; and (3) amorphous hydrogenated carbon nitride grown from volatile organic precursors (allylamine, acetonitrile). In the three cases, X-ray photoelectron spectroscopy (XPS) results show that chemisorption of the catalyst occurs on the nitrogen-containing functionalities created by plasma polymerization and grafting and thus that the electroless deposition is possible. Differences were observed depending on the nature and thickness of the plasma-polymerized thin films, as well as on the nature and concentration of the nitrogen-containing functionalities present or grafted at the surface. Practical adhesion of Ni films was investigated using a Scotch(R) tape test. Ni films up to 3 or 4 mum in thickness were shown to pass this test successfully, i.e., without causing any metal detachment.