An isotope-doped carbon nanotube (40) includes at least two kinds of carbon nanotube segments, each kind of carbon nanotube segment having a unique carbon isotope. The at least two kinds of carbon nanotube segments are arranged along a longitudinal direction of the carbon nanotube alternately or non-alternately. The carbon isotope is selected from the group consisting of a carbon-12 isotope, a carbon-13 isotope and a carbon-14 isotope. Three preferred methods employ different single isotope sources to form isotope-doped carbon nanotubes. In a chemical vapor deposition method, different isotope source gases are alternately or non-alternately introduced. In an arc discharge method, a power source is alternately or non-alternately switched between different isotope anodes. In a laser ablation method, a laser is alternately or non-alternately focused on different isotope targets.