The fabrication and filling of carbon nanomaterials (CNMs) into nanoholes and trenches using supercritical method were achieved for the first time at substrate temperatures of 500–700 °C and pressures of 10–20 MPa. Two supercritical fluid systems were examined: (1) ethanol and carbon dioxide were used as the carbon source and supercritical fluid, respectively, and (2) ethanol was used as both the carbon source and supercritical fluid. Multiwalled carbon nanotubes with diameters of 8–20 nm were also confirmed to be formed. The present work introduces a new technique of preparing CNMs for application as large-scale integration interconnects.