A novel fabrication of two-dimensional CdTe nanoarchitecture was developed through the interaction between bolaamphiphiles of 1,3-bis(hexadecyldimethylammonio)propane dibromide and the prepared negatively charged CdTe nanocrystals hydrosols by controlling the surface pressure of the monolayer. The formed amphiphiles/CdTe nanocrystals composite monolayer confirm that plenty of CdTe nanorod-like nanostructure with the lengths of roughly 100-300 nm and the widths of about 25-nm distribute in Langmuir layer by a self-assembly way at low surface pressure.