A study has been made of the carbon formation in the surface layer of Ag-, W- and Pd-ions implanted polyimide films. The doses of 130 KeV Ag-ions and 190 KeV W-ions ranged from lxlO16 to 5×1017 atoms/cm2. The doses of 100 KeV Pd-ions ranged from 5×1016 to 2×1017 atoms/cm2. The carbon structure in implanted layers was characterized by laser Raman spectroscopy (LRS). Non-implanted polyimide film has very strong intensity of fluorescence, and the intensity of all W-, Ag- and Pd-ions implanted specimens decreases with the increase in dose. The intensity of Raman spectra for both W- and Ag-ions implanted specimens increases with the increase in dose. For Pd-ion implanted specimens, the Raman spectrum of carbon is hardly observed even with a high dose. Raman spectra for W- or Ag-ions implanted specimens with a high dose show that the diamond-like carbon (DLC) exist in the implanted layers. It is found that the DLC structures in the W- and Ag-ions implanted layers have graphite-like and amorphous-like structures, respectively. We propose that transparency carbon structure in implanted layers is generated by Pd-ion implantation. It is concluded that marked DLC formation in surface layer of polyimide films can be caused by Ag- or W-ions implantation except Pd-ion implantation, and carbon structure in implanted layers depends strongly on the implanted elements.