A method of fabricating nanocrystal tubules was developed by coating carboxylic acid--thiol capped Au nanocrystals on peptide tubule templates to form the Au nanocrystal tubules, Hydrogen bonding between the amide groups of the tubules and the carboxylic acid groups of the nanocrystals was used as a driving force for this assembly process. The Au nanocrystal tubules with hollow structures were applied to hold and analyze trace molecules as signal-enhancing cuvettes for Raman spectroscopy. The Raman scattering of trace Rhodamine B on the Au nanocrystal-coated tubule was enhanced by a factor of 10(5).