A systematic investigation on the unusual attachment of labile deuterium to carbon nanotubes in deuterated water and alcohols is reported. The carbon nanotubes were solubilized through the established functionalization of the nanotube-bound carboxylic acids to allow solution-phase reaction and characterization. The deuterium attachment was found under several experimental conditions, including the use of deuterated ethanol as a co-reactant in the nanotube functionalization reaction and the refluxing of functionalized or simply purified carbon nanotubes in deuterated water and alcohols. The solubility of the functionalized carbon nanotube samples in common organic solvents and water allowed unambiguous H-2 NMR characterization. The reproducible broad H-2 NMR signal at similar to6.5 ppm is assigned to carbon nanotube-attached deuterium species. The assignment is supported by the results from FT-IR measurements. The carbon-deuterium interaction is so strong that the corresponding vibration resembles the typical C-D stretching mode in the characteristic frequency region. The FT-IR peak intensities also correlate well with the H-2 NMR signal integrations in a series of samples. Mechanistic implications of the results are discussed.