The specimens were characterized by field emission scanning electron microscopy, atomic force microscopy, and mechanical pull-up tests. A noticed relationship between the implanted voltage and the nanostructure of the implanted Cu was established. The effects of the implanted nanostructure related to the adhesion strength of the electroless-plated Cu film were discussed. The adhesion strength of the final electroless-plated Cu film followed with the implanted dosage of 10 × 1016 cm−2 is apparently higher than that with the dosage of 5.0 × 1016 cm−2 at the same accelerating voltage. The adhesion strength of the Cu films tends to decrease with the increasing accelerating voltages applied for the implantation. An excellent gap-filling capability in a 0.2 μm width (aspect ratio 7:1) via was obtained.